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Su, Yu-Sheng, Kuang-Che Hsiao, Pedaballi Sireesha, and Jen-Yen Huang. "Lithium Silicates in Anode Materials for Li-Ion and Li Metal Batteries." Batteries 8, no. 1 (January 4, 2022): 2. http://dx.doi.org/10.3390/batteries8010002.
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The structural and interfacial stability of silicon-based and lithium metal anode materials is essential to their battery performance. Scientists are looking for a better inactive material to buffer strong volume change and suppress unwanted surface reactions of these anodes during cycling. Lithium silicates formed in situ during the formation cycle of silicon monoxide anode not only manage anode swelling but also avoid undesired interfacial interactions, contributing to the successful commercialization of silicon monoxide anode materials. Additionally, lithium silicates have been further utilized in the design of advanced silicon and lithium metal anodes, and the results have shown significant promise in the past few years. In this review article, we summarize the structures, electrochemical properties, and formation conditions of lithium silicates. Their applications in advanced silicon and lithium metal anode materials are also introduced.
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Yang, Chunpeng, Lei Zhang, Boyang Liu, Shaomao Xu, Tanner Hamann, Dennis McOwen, Jiaqi Dai, et al. "Continuous plating/stripping behavior of solid-state lithium metal anode in a 3D ion-conductive framework." Proceedings of the National Academy of Sciences 115, no. 15 (March 26, 2018): 3770–75. http://dx.doi.org/10.1073/pnas.1719758115.
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The increasing demands for efficient and clean energy-storage systems have spurred the development of Li metal batteries, which possess attractively high energy densities. For practical application of Li metal batteries, it is vital to resolve the intrinsic problems of Li metal anodes, i.e., the formation of Li dendrites, interfacial instability, and huge volume changes during cycling. Utilization of solid-state electrolytes for Li metal anodes is a promising approach to address those issues. In this study, we use a 3D garnet-type ion-conductive framework as a host for the Li metal anode and study the plating and stripping behaviors of the Li metal anode within the solid ion-conductive host. We show that with a solid-state ion-conductive framework and a planar current collector at the bottom, Li is plated from the bottom and rises during deposition, away from the separator layer and free from electrolyte penetration and short circuit. Owing to the solid-state deposition property, Li grows smoothly in the pores of the garnet host without forming Li dendrites. The dendrite-free deposition and continuous rise/fall of Li metal during plating/stripping in the 3D ion-conductive host promise a safe and durable Li metal anode. The solid-state Li anode shows stable cycling at 0.5 mA cm−2 for 300 h with a small overpotential, showing a significant improvement compared with reported Li anodes with ceramic electrolytes. By fundamentally eliminating the dendrite issue, the solid Li metal anode shows a great potential to build safe and reliable Li metal batteries.
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Park, Se Hwan, Dayoung Jun, Gyu Hyeon Lee, Seong Gyu Lee, Ji Eun Jung, and Yun Jung Lee. "Designing the 3D Porous Anode Based on Pore Size Dependent Li Deposition Behavior for Reversible Li Metal-Free Solid-State-Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 470. http://dx.doi.org/10.1149/ma2022-024470mtgabs.
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Li metal-based all-solid-state batteries (ASSBs) can potentially combine the high energy of Li metal anodes and the safety of ASSBs. Among Li metal-based ASSBs, lithium-free or anodeless ASSBs are considered optimal battery configurations because of their higher energy density and economic advantages attributed to the absence of Li metal during the battery assembly process. Despite the extensive interest in Li-free ASSBs, they continue to suffer from low Coulombic efficiency and poor cycle performance. One reason for this inferior performance is the unstable interface between the current collector and solid electrolyte (SE), which can eventually lead to inhomogeneous Li deposition, dendritic Li growth, and internal short circuits. Various approaches including 3D porous anodes have been proposed to control the Li deposition behavior and improve the reversibility of anodeless ASSBs; however, there is no clarity on the mechanism and conditions for determining the Li deposition behavior in this emerging system. In this study, we systematically investigate the Li deposition behavior depending on the pore size of 3D anode and successfully demonstrate the strategy to obtain a highly reversible 3D porous anode for Li-free ASSBs. We found that more Li deposits could be accommodated within the pores of the anode with a smaller pore size using stacked Ni particles as the Li-hosting porous anode; this implies that the Li movement into the anode occurs via diffusional Coble creep. We proposed the modification of the Ni surface with carbon coating and Ag nanoparticle decoration (Ni_C_Ag particles) to further improve the Li storage capacity of the Ni-based 3D anode and, thereby, secure the interfacial contact between the 3D Ni anode and SE. The resulting Ni_C_Ag 3D anode successfully accommodated the entire Li deposit of 2 mAh cm−2 within the porous architecture without the separation of the anode/SE interface. We clarified the improved Li storage capacity of the Ni_C_Ag anode as follows. (1) C and especially Ag electrochemically react with Li ions above 0 V; thus, Li ions can be transported to 3D Ni_C_Ag porous anode before Li deposition at the SE/anode interface at < 0 V. Further, the high Li ion diffusion coefficient of lithiated carbon and Li-Ag alloy can further reduce Li ions within the pores of the 3D anode; therefore, Li deposition can occur within the porous 3D Ni anode. (2) Lithiophilic C and Ag facilitated the movement of Li via diffusional Coble creep. In particular, Ag with solid solubility in Li (Li(Ag)) can significantly enhance Li adatom mobility because of the identical structure of Li(Ag) with pure Li. (3) Li(Ag) is widely known to lower the energy barrier for Li nucleation. With the significantly reduced nucleation overpotential and interfacial resistance, the Ni_C_Ag anode showed high reversibility in Li deposition and stripping. The Ni_C_Ag anode could be cycled for more than 60 and 100 cycles with Li3PS4 and Li6PS5Cl0.5Br0.5 SE in half cells with a capacity limit of 2 mAh cm−2 and a current density of 0.5 mA cm− 2maintaining the CE of 97.9% and 96.9 %, respectively. Further, the synergistic effects of the stable anode/SE interface and reduced nucleation energy barrier enable stable NCM full-cell cycling at a room temperature of 30 °C. The NCM811 cathode/Ni_C_Ag anode full cell in the Li-free configuration showed an initial areal discharge capacity of 2 mAh cm−2, and it operated stably with a CE of 99.47% for 100 cycles. Figure 1
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Bao, Wurigumula, and Ying Shirley Meng. "(Invited) Development and Application of Titration Gas Chromatography in Elucidating the Behavior of Anode in Lithium Batteries." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 633. http://dx.doi.org/10.1149/ma2023-012633mtgabs.
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The accelerated transition to renewable energy systems worldwide has triggered increasing interest in energy storage technologies, especially in lithium batteries. Accurate diagnosis and understanding of the batteries degradation mechanism are essential. Titration Gas Chromatography (TGC) has been developed to quantitively understand the anode. The inactive Li in the cycled anode can be categorized into two kinds: 1) trapped Li0 (such as trapped lithiated graphite (LixC6), Li0, and lithium silicon alloy (LixSi)) and 2) solid electrolyte interphase (SEI) Li+. Noted that only trapped Li0 can react with the protic solvent to generate the hydrogen (H2), while SEI (Li+) does not1. Therefore, the H2 gas quantification can be correlated to the trapped Li0 as the foundation mechanism of TGC. With the optimal solvent selection, we successfully applied TGC to investigated: 1) the degradation behavior of Si-based anode materials2, 3; 2) corrosion effects on electrochemically deposited Li metal anode4; 3) the cycling behavior of Gr anode; 4) Li inventory quantification in practical Li metal battery5. We demonstrate the various application of TGC techniques in quantitatively examining the Li inventory changes of the anode. Beyond that, the results can provide unique insights into identifying the critical bottlenecks that facilitate battery performance development. References: Fang, C.; Li, J.; Zhang, M.; Zhang, Y.; Yang, F.; Lee, J. Z.; Lee, M. H.; Alvarado, J.; Schroeder, M. A.; Yang, Y.; Lu, B.; Williams, N.; Ceja, M.; Yang, L.; Cai, M.; Gu, J.; Xu, K.; Wang, X.; Meng, Y. S., Quantifying inactive lithium in lithium metal batteries. Nature 2019, 572 (7770), 511-515. Bao, W.; Fang, C.; Cheng, D.; Zhang, Y.; Lu, B.; Tan, D. H.; Shimizu, R.; Sreenarayanan, B.; Bai, S.; Li, W., Quantifying lithium loss in amorphous silicon thin-film anodes via titration-gas chromatography. Cell Reports Physical Science 2021, 2 (10), 100597. Sreenarayanan, B.; Tan, D. H.; Bai, S.; Li, W.; Bao, W.; Meng, Y. S., Quantification of lithium inventory loss in micro silicon anode via titration-gas chromatography. Journal of Power Sources 2022, 531, 231327. Lu, B.; Li, W.; Cheng, D.; Bhamwala, B.; Ceja, M.; Bao, W.; Fang, C.; Meng, Y. S., Suppressing chemical corrosions of lithium metal anodes. Advanced Energy Materials 2022, 2202012. Deng, W.; Yin, X.; Bao, W.; Zhou, X.; Hu, Z.; He, B.; Qiu, B.; Meng, Y. S.; Liu, Z., Quantification of reversible and irreversible lithium in practical lithium-metal batteries. Nature Energy 2022, 7 (11), 1031-1041.
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Wang, Hansen, Yayuan Liu, Yuzhang Li, and Yi Cui. "Lithium Metal Anode Materials Design: Interphase and Host." Electrochemical Energy Reviews 2, no. 4 (October 12, 2019): 509–17. http://dx.doi.org/10.1007/s41918-019-00054-2.
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Abstract Li metal is the ultimate anode choice due to its highest theoretical capacity and lowest electrode potential, but it is far from practical applications with its poor cycle lifetime. Recent research progresses show that materials designs of interphase and host structures for Li metal are two effective ways addressing the key issues of Li metal anodes. Despite the exciting improvement on Li metal cycling capability, problems still exist with these methodologies, such as the deficient long-time cycling stability of interphase materials and the accelerated Li corrosion for high surface area three-dimensional composite Li anodes. As a result, Coulombic efficiency of Li metal is still not sufficient for full-cell cycling. In the near future, an interphase protected three-dimensional composite Li metal anode, combined with high performance novel electrolytes might be the ultimate solution. Besides, nanoscale characterization technologies are also vital for guiding future Li metal anode designs. Graphic Abstract
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Gabrisch, H., R. Yazami, and B. Fultz. "Lattice defects in LiCoO2." Microscopy and Microanalysis 7, S2 (August 2001): 518–19. http://dx.doi.org/10.1017/s143192760002866x.
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Rechargeable Lithium ion batteries are widely used as portable power source in communication and computer technology, prospective uses include medical implantable devices and electric vehicles. The safety and cycle life of Li ion batteries is improved over that of batteries containing metallic lithium anodes because the insertion of Li between the crystal layers of both electrodes was proved to be safer than the electroplating of Li onto a metallic Lithium anode. in Li-ion batteries, the charge transport is governed by the oscillation of Li ions between anode and cathode. They are sometimes called “rocking-chair“ batteries. The most common materials for these batteries are lithiated carbons for anodes, and transition metal oxides (LixCoO2) as cathodes.LixCoO2 has an ordered rhombohedral Rm structure consisting of alternating layers of Co-O-Li-O-Co. The capacity and energy density of the batteries is limited by the amount of Li that can be stored in the anode and cathode materials.
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Fluegel, Marius, Karsten Richter, Margret Wohlfahrt-Mehrens, and Thomas Waldmann. "Detection of Li Deposition on Si/Graphite Anodes from Commercial Li-Ion Cells - a Post-Mortem GD-OES Depth Profiling Study." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 239. http://dx.doi.org/10.1149/ma2022-023239mtgabs.
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A new semi-quantitative method based on Post-Mortem glow discharge optical emission spectroscopy (GD-OES) depth profiling was developed to detect Li deposition on Si/graphite anodes. By means of the detected amounts of Li, Si and O in the GD-OES depth profiles, a corridor is determined, in which the minimum amount of Li deposition is found. Three different commercially available 18650 cell types containing Si/graphite as anode active material were acquired to evaluate the newly developed method. Those three cell types were initially characterized in detail by means of SEM/EDX, GD-OES, ICP-OES, and Hg porosimetry regarding their cell chemistry and electrode properties. One cell type was a high-power cell due to its high anode porosity and low anode coating thickness. The other two cell types were high-energy cells, which have thick anode coatings and low porosities. We aged the cells at 45 °C until their SOH was 80% and analysed the aging behaviour using SEM, DVA, GD-OES, and in coin half-cells. GD-OES depth profiling revealed that no Li plating occurs during cycling aging at 45 °C. Contrary to this, Li plating was detected on the anodes of all three cell types by the new GD-OES method after the high-power cell was aged at -20 °C and the high-energy cells were aged to 0 °C. Cells, which were previously aged at 45 °C until 80% SOH have afterwards been cycled under the same conditions, which led to Li plating in the fresh cells. Cell types exhibiting predominantly loss of anode active material (LAAM) as aging mechanism during the first aging at 45 °C, still suffered from Li plating during the second aging. However, if the main aging mechanism during the initial aging was loss of cyclable Li inventory (LLI), the cells did show a significantly reduced tendency for Li plating, even though the same conditions caused Li plating in the fresh cells. Analysis of the aged anodes using coin half-cells revealed that the loss of anode material was caused by the deactivation of Si anode material. SEM images of the anode cross-section indicate that the deactivation is most likely mainly induced by the formation of a thick film surrounding the Si particles. In combination with complementary methods like SEM, ICP-OES, and coin half-cell analysis, the newly developed GD-OES method yields in profound understanding of the aging behaviour of state-of-the-art Li-ion cells contain Si/graphite anodes. Figure 1
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Dasgupta, Neil P. "(Invited) Interfacial Dynamics of Anode-Free Solid-State Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 482. http://dx.doi.org/10.1149/ma2022-024482mtgabs.
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There is significant interest in solid-state batteries (SSBs) as an alternative to traditional Li-ion batteries, as they can potentially eliminate the flammable liquid electrolyte and enable Li-metal anodes. However, manufacturing of SSBs with Li metal anodes poses a significant challenge, owing to the highly reactive nature of Li metal. Therefore, there has been a recent increase in interest in “anode-free” configurations, where the Li metal anode is formed in situ using the pre-existing inventory in the cathode. In addition to manufacturing considerations, anode-free configurations also enhance energy density compared to batteries with excess Li metal in the anode. However, compared to pre-formed Li metal/solid electrolyte interfaces, the nucleation, growth, and stripping of Li metal in anode-free SSBs has not been widely studied, and poses unique electro-chemo-mechanical phenomena. To probe the dynamic interfacial evolution of anode-free SSBs, in this study, I will present results using a complimentary set of in situ/operando methodologies. First, I will describe the morphological evolution of Li nucleation and growth at garnet LLZO solid electrolytes, using a newly developed platform for operando 3-D video microscopy [1]. In particular, the influence of mechanical stresses on both the thermodynamic and kinetic properties of Li will be discussed, and unique electrochemical signatures of anode-free plating will described. A mechanistic framework for these electro-chemo-mechanics will be presented, which results in design rules for improving the homogeneity of Li plating during anode formation. To compliment this morphological information, I will also present results using operando x-ray photoelectron spectroscopy (XPS) on sulfide solid electrolytes. This allows for direct observation of SEI formation during in situ anode formation. In particular, we observe a transition in reaction pathways from SEI formation to nucleation of Li metal, which is a function of both the charging protocol and the presence of interlayer coatings [2-3]. Finally, these results will be compared and contrasted to anode-free Li plating in liquid electrolytes, and a discussion will be presented on how to optimize plating morphology and reversibility. [1] E. Kazyak, M. Wang, K. Lee, S. Yadavalli, A. J. Sanchez, M. D. Thouless, J. Sakamoto, N. P. Dasgupta, Submitted (2022). [2] A. L. Davis, R. Garcia-Mendez, K. N. Wood, E. Kazyak, K.-H. Chen, G. Teeter, J. Sakamoto, N. P. Dasgupta, J. Mater. Chem. A 8, 6291 (2020). [3] A. L. Davis, E. Kazyak, D. W. Liao, K. N. Wood, N. P. Dasgupta, J. Electrochem. Soc. 168, 070557 (2021).
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Zhao, Nahong, Lijun Fu, Lichun Yang, Tao Zhang, Gaojun Wang, Yuping Wu, and Teunis van Ree. "Nanostructured anode materials for Li-ion batteries." Pure and Applied Chemistry 80, no. 11 (January 1, 2008): 2283–95. http://dx.doi.org/10.1351/pac200880112283.
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This paper focuses on the latest progress in the preparation of a series of nanostructured anode materials in our laboratory and their electrochemical properties for Li-ion batteries. These anode materials include core-shell structured Si nanocomposites, TiO2 nanocomposites, novel MoO2 anode material, and carbon nanotube (CNT)-coated SnO2 nanowires (NWs). The substantial advantages of these nanostructured anodes provide greatly improved electrochemical performance including high capacity, better cycling behavior, and rate capability.
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Meng, Shirley. "Understanding Li Nucleation and Growth." ECS Meeting Abstracts MA2023-01, no. 22 (August 28, 2023): 1580. http://dx.doi.org/10.1149/ma2023-01221580mtgabs.
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Lithium metal anode has been widely studied for next generation lithium metal batteries. Its chemical, electrochemical and mechanical properties are unique as lithium is the lightest metal in the planet earth. In this talk, I will use some of the advanced modeling and characterization methods to probe and understand the lithium metal anode in a rechargeable battery. The tools we developed here will be also useful for other reactive metal anodes such as sodium and zinc.
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Suh, Joo Hyeong, Dong Ki Kim, and Min-Sik Park. "Perspectives on the development of advanced lithium metal anode." Ceramist 26, no. 2 (June 30, 2023): 265–79. http://dx.doi.org/10.31613/ceramist.2023.26.2.08.
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The demand for high-energy Li batteries is rapidly increasing due to the growing market for electric vehicles and portable electronic devices. Lithium (Li) metal has been considered as an ideal anode for high-energy Li batteries because of its high theoretical capacity (3860 mAh g<sup>-1</sup>) and low redox potential (-3.04 V vs. SHE). However, the utilization of Li metal anode is still limited by fundamental problems associated with unavoidable dendritic growth and huge volume changes during cycling. To improve the electrochemical performance of Li metal anode, various strategies have been explored including electrolyte design, interfacial engineering, and structural modifications. One of the most promising approaches is to store Li metal in porous host materials, which can effectively suppress the formation of Li dendrite and volume expansion. Herein, we focus on recent progress in the development of advanced Li metal anodes and suggest research directions and design rules.
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Flügel, Marius, Karsten Richter, Margret Wohlfahrt-Mehrens, and Thomas Waldmann. "Detection of Li Deposition on Si/Graphite Anodes from Commercial Li-Ion Cells: A Post-Mortem GD-OES Depth Profiling Study." Journal of The Electrochemical Society 169, no. 5 (May 1, 2022): 050533. http://dx.doi.org/10.1149/1945-7111/ac70af.
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A new semi-quantitative method was developed to detect Li deposition on Si/graphite anodes. This method is based on Post-Mortem glow discharge optical emission spectroscopy (GD-OES) depth profiling. Based on the contents of Si, Li, and O in the GD-OES depth profiles, we define a corridor, in which the minimum amount of metallic Li on the anode is located. This method was applied to three types of commercial 18650 cells with Si/graphite anodes in the fresh state and with Li plating intentionally produced by cycling at low temperatures. Additional cells were cycling aged at 45 °C to 80% SOH. The main aging mechanisms at 45 °C were determined using differential voltage analysis (DVA), SEM, and half cell experiments. Subsequently, the cells aged at 45 °C were further cycled under the conditions that had led to Li deposition for the fresh cells. Furthermore, the anode coating thickness for 18 types of commercial Li-ion cells are correlated with the specific energy, while distinguishing between graphite anodes and Si/graphite anodes. Our extensive Post-Mortem study gives deep insights into the aging behavior of state-of-the-art Li-ion cells with Si/graphite anodes.
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Wang, Jian, Yuan Chen, and Lu Qi. "The Development of Silicon Nanocomposite Materials for Li-Ion Secondary Batteries." Open Materials Science Journal 5, no. 1 (December 2, 2011): 228–35. http://dx.doi.org/10.2174/1874088x01105010228.
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With the rapid progress and wide application of Li-ion batteries, commercial graphite anode can not satisfy the increasing demand for higher capacities. Like other anode materials with higher capacities, silicon materials as anodes remain serious problems for their large volume variations and poor cyclabilities during cycling. One of key problem is how to stabilize the performances of Si anode materials. Various influencing factors of volume variation of silicon anode materials have been reviewed, which consist of discharging voltage, amorphous or crystalline type, tube or pore microstructure, interlayer adhesion, buffering and protective layer materials and conductive agents. Another hot issue is on the preparation methods for silicon anode materials with high performance. It covers not only the technics of high purity silicon materials, including the predominant Siemens process of electronic-grade silicon, but also the techniques of silicon film anodes, which consists of butyl-capped silicon precursor, the template methods of nanostructure, magnetron sputtering, ball-milling. From the screening of existing silicon anode materials in the literatures, the preparation methods for promising Si anode materials and their prospects have been offered.
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Kolosov, Dmitry A., and Olga E. Glukhova. "Theoretical Study of a New Porous 2D Silicon-Filled Composite Based on Graphene and Single-Walled Carbon Nanotubes for Lithium-Ion Batteries." Applied Sciences 10, no. 17 (August 21, 2020): 5786. http://dx.doi.org/10.3390/app10175786.
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The incorporation of Si16 nanoclusters into the pores of pillared graphene on the base of single-walled carbon nanotubes (SWCNTs) significantly improved its properties as anode material of Li-ion batteries. Quantum-chemical calculation of the silicon-filled pillared graphene efficiency found (I) the optimal mass fraction of silicon (Si)providing maximum anode capacity; (II) the optimal Li: C and Li: Si ratios, when a smaller number of C and Si atoms captured more amount of Li ions; and (III) the conditions of the most energetically favorable delithiation process. For 2D-pillared graphene with a sheet spacing of 2–3 nm and SWCNTs distance of ~5 nm the best silicon concentration in pores was ~13–18 wt.%. In this case the value of achieved capacity exceeded the graphite anode one by 400%. Increasing of silicon mass fraction to 35–44% or more leads to a decrease in the anode capacity and to a risk of pillared graphene destruction. It is predicted that this study will provide useful information for the design of hybrid silicon-carbon anodes for efficient next-generation Li-ion batteries.
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Son, Yeonguk, Taeyong Lee, Bo Wen, Jiyoung Ma, Changshin Jo, Yoon-Gyo Cho, Adam Boies, Jaephil Cho, and Michael De Volder. "High energy density anodes using hybrid Li intercalation and plating mechanisms on natural graphite." Energy & Environmental Science 13, no. 10 (2020): 3723–31. http://dx.doi.org/10.1039/d0ee02230f.
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Shen, Yi Yang. "MoS2/Graphene Heterostructure Anode for Li-Ion Battery Application: A First-Principles Study." Key Engineering Materials 896 (August 10, 2021): 53–59. http://dx.doi.org/10.4028/www.scientific.net/kem.896.53.
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The development of next generation Li ion battery has attracted many attentions of researchers due to the rapidly increasing demands to portable energy storage devices. General Li metal/alloy anodes are confronted with challenges of dendritic crystal formation and slow charge/discharge rate. Recently, the prosperity of two-dimensional materials opens a new window for the design of battery anode. In the present study, MoS2/graphene heterostructure is investigate for the anode application of Li ion battery using first-principles calculations. The Li binding energy, open-circuit voltage, and electronic band structures are acquired for various Li concentrations. We found the open-circuit voltage decreases from ~2.28 to ~0.4 V for concentration from 0 to 1. Density of states show the electrical conductivity of the intercalated heterostructures can be significantly enhanced. The charge density differences are used to explain the variations of voltage and density of states. Last, ~0.43 eV diffusion energy barrier of Li implies the possible fast charge/discharge rate. Our study indicate MoS2/graphene heterostructure is promising material as Li ion battery anode.
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Yu, Han, Jian Xie, Na Shu, Fei Pan, Jianglin Ye, Xinyuan Wang, Hong Yuan, and Yanwu Zhu. "A Sponge-Driven Elastic Interface for Lithium Metal Anodes." Research 2019 (September 15, 2019): 1–10. http://dx.doi.org/10.34133/2019/9129457.
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The lithium (Li) metal is one promising anode for next generation high-energy-density batteries, but the large stress fluctuation and the nonuniform Li deposition upon cycling result in a highly unstable interface of the Li anode. Herein, a simple yet facile engineering of the elastic interface on the Li metal anodes is designed by inserting a melamine sponge between Li and the separator. Driven by the good elasticity of the sponge, the modified Li anode maintains a Coulombic efficiency of 98.8% for 60 cycles and is cyclable at 10 mA cm-2 for 250 cycles, both with a high capacity of 10 mA h cm-2. We demonstrate that the sponge can be used to replace the conventional polypropylene as a porous yet elastic separator, showing superior cycling and rate performance as well. In addition to the efficiency of the elastic interface on the cycling stability, which is further confirmed by an in situ compression-electrochemistry measurement, the porous structure and polar groups of the sponge demonstrate an ability of regulating the transport of Li ions, leading to a uniform deposition of Li and the suppression of Li dendrites in cycling.
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Tang, Shuai, Xiang Li, Qianqian Fan, Xiuqing Zhang, Dan-Yang Wang, Wei Guo, and Yongzhu Fu. "Review—Advances in Rechargeable Li-S Full Cells." Journal of The Electrochemical Society 169, no. 4 (April 1, 2022): 040525. http://dx.doi.org/10.1149/1945-7111/ac638c.
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Lithium sulfur (Li-S) batteries with the high theoretical specific energy of 2600 Wh kg−1 are a promising candidate at the era of the post lithium-ion batteries. In most studies, lithium metal anode is used. To advance the Li-S battery towards practical application, Li-S full cells with low or non-Li metal anode need to be developed. Herein, the latest advances of the Li-S full cells are mainly categorized according to the initial state of the S cathode, i.e., sulfur (S) and lithium sulfide (Li2S). In each part, the challenges and strategies are thoroughly reviewed for the cells with different anodes, such as carbon, silicon, other alloys and metallic Li. The cycling performance comparisons of state-of-the-art Li-S full cells are also included. To achieve the high real energy density for practical applications, the Li-S full cells have to use low excess lithiated graphite, lithiated alloys, or metallic Li as the anodes. Meanwhile, the lean electrolyte is also important to further improve the practical energy density. The review is expected to supply a comprehensive guide to design Li-S full cells.
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Zhang, Wenjie, Siming Yang, Shuai Heng, Ximei Gao, Yan Wang, Wenxiang Zhang, Qunting Qu, and Honghe Zheng. "Improved solid electrolyte interphase and Li-storage performance of Si/graphite anode with ethylene sulfate as electrolyte additive." Functional Materials Letters 13, no. 07 (October 2020): 2051041. http://dx.doi.org/10.1142/s1793604720510418.
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Silicon/graphite composite anodes have drawn extensive attention in the field of power Li-ion batteries for application in electric vehicles because of their much higher capacity than that of traditional graphite anodes. In this work, ethylene sulfate (1,3,2-dioxathiolane-2,2-dioxide, DTD) is investigated as an electrolyte additive to improve the Li-storage performance of silicon/graphite composite anode. The electrochemical behavior of silicon/graphite anode including cyclic voltammogram, discharge/charge performance at various current density and during long-term cycling, and electrochemical impedance is systematically studied by adding different amounts of DTD into electrolyte. The effects of DTD on the solid/electrolyte interphase (SEI) film are analyzed through scanning electron microscopy, X-ray photoelectron and Fourier transform infrared spectroscopy. It is found that DTD participates into the film-formation process through its reductive decomposition reactions on electrode surface, producing a thin, uniform and stable SEI. The Li-storage performance of silicon/graphite anode is improved at an optimized addition amount of DTD.
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Wood, Marissa, Yiran Xiao, Megan C. Freyman, Bo Wang, Cheng Zhu, and Sichi Li. "Designing Better Li Metal Anodes for Solid-State Batteries Using a Combined Experiment/Theory Approach." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 781. http://dx.doi.org/10.1149/ma2023-024781mtgabs.
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Solid-state batteries have the potential to transform energy storage by providing significantly higher energy densities and improved safety compared to conventional Li-ion batteries. Robust high-capacity Li metal anodes are necessary to realize this technology, but current Li metal anode designs suffer from significant degradation over time due to non-uniform Li plating/stripping and loss of contact with the solid electrolyte during cycling. Carbon scaffold hosts have been shown to mitigate this problem in liquid electrolyte systems by creating a uniform electric field and providing abundant Li nucleation sites, but they have not been well explored in solid-state systems, which require the fabrication of more complicated mixed ion/electron conducting scaffolds to provide transport of both Li ions and electrons throughout the anode. We investigated the effect of scaffold architecture and chemistry on the resulting Li morphology and electrochemical performance using a combined experiment/theory approach. Carbon scaffolds with well-controlled geometries and varied porosities were fabricated using 3D printing and then characterized by SEM, Raman, and XPS before cycling in cells to evaluate their performance as hosts for uniform Li plating/stripping. Atomistic and mesoscale modeling were used to predict how scaffold chemistry and microstructure affect Li nucleation probability and the formation of current density/stress hotspots that can lead to dendrite growth, and these results were used to help guide scaffold design. This work provides further insight into the relationship between anode architecture and Li metal cycling stability in solid-state batteries and demonstrates progress toward an anode-free configuration, which promises to simplify cell manufacturing, decrease cost, and increase energy density by plating the Li metal anode directly from the cathode in situ. Lawrence Livermore National Laboratory is operated by Lawrence Livermore National Security, LLC, for the U.S. Department of Energy, National Nuclear Security Administration under Contract DE-AC52-07NA27344.
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Kazyak, Eric, Srinivas Yadavalli, Kiwoong Lee, Michael Wang, Adrian J. Sanchez, M. D. Thouless, Jeff Sakamoto, and Neil P. Dasgupta. "Understanding Coupled Electro-Chemo-Mechanics during I n Situ Li Metal Anode Formation in Anode-Free Solid-State Batteries." ECS Meeting Abstracts MA2022-01, no. 37 (July 7, 2022): 1630. http://dx.doi.org/10.1149/ma2022-01371630mtgabs.
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Solid-state batteries (SSBs) are potentially disruptive for a range of applications owing to their promise of high energy density, improved safety, and long cycle life. Their ability to enable Li metal anodes is a major advantage for energy density, but Li presents challenges for manufacturing due to its reactivity and the difficulty of fabricating thin Li films and high-quality Li/Electrolyte interfaces. Recently, in situ anode formation has shown significant promise for overcoming these challenges. In this approach, the cells are assembled without an anode (“Anode-free”), and Li metal is plated out from the cathode after fabrication. This reduces the need for inert atmospheres and reduces cell complexity, potentially lowering cost. As Li is plated out for the first time, mechanical stresses evolve at the Li/Electrolyte interface due to the volumetric changes in the electrodes. These stresses and the coupling between mechanics and electrochemistry play an important role in the resulting uniformity and quality of the in situ formed Li electrode. This work leverages 3D operandooptical video microscopy to observe morphology changes during in situ anode formation on one of the most promising solid electrolytes, Li7La3Zr2O12 (LLZO). These morphology changes are linked to the electrochemical signatures and the dynamic evolution of mechanical stresses at the Li/LLZO interface. A mechanistic framework is built to understand these factors, which is then used to provide guidance on what parameters control uniformity, and how systems can be designed to improve the resulting electrode properties. The role of stack pressure and the importance of stack pressure uniformity is highlighted. The impact of interfacial toughness, current collector properties, and cell geometry are discussed. Based on this understanding, the areal Li coverage is improved by more than 50%, providing insight for future works to enable in situ anode formation in a range of material systems and cell architectures.
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Choi, Yusong, Jaein Lee, Tae-Young Ahn, and Sang-Hyeon Ha. "Highly Lithiophilic Oxidative Interfacial Layer for 3D Foam-Based Lithium Metal Anode: Lithium Impregnated Metal Foam Anode (LIMFA)." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 311. http://dx.doi.org/10.1149/ma2023-022311mtgabs.
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Numerous lithium-infused (or impregnated) lithium-metal anodes using pure Ni foams with excellent properties have been developed for use in Li batteries. However, pure Ni exhibits high reactivity with molten Li during infusion (e.g., coating, impregnation, etc.). Herein, a high-performance and ultra-stable (against molten Li) lithium-impregnated metal foam anode (LIMFA) is fabricated by a simple oxidation of nickel based alloy foam at 900 °C in air. A symmetric cell test employing the LIMFA anode showed stable stripping and plating performance. For thermal batteries without cup, LIMFA provided the highest reported specific capacity and first discharge of molten Li. After the cell discharge, the Ni based foam exhibited no Li leakage, surface damage, or structural collapse. Given these advantageous properties, in addition to its high specific capacity, LIMFA is expected to aid in the development of thermal batteries with enhanced performance.
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Flügel, Marius, Marius Bolsinger, Mario Marinaro, Volker Knoblauch, Markus Hölzle, Margret Wohlfahrt-Mehrens, and Thomas Waldmann. "Onset Shift of Li Plating on Si/Graphite Anodes with Increasing Si Content." Journal of The Electrochemical Society 170, no. 6 (June 1, 2023): 060536. http://dx.doi.org/10.1149/1945-7111/acdda3.
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Mixing graphite with Si particles in anodes of Li-ion batteries provides increased specific energy. In addition, higher Si contents lead to thinner anode coatings at constant areal capacity. In the present study, we systematically investigated the influence of the Si content on the susceptibility of Li plating on Si/graphite anodes. Si/graphite anodes with Si contents from 0 to 20.8 wt% combined with NMC622 cathodes were manufactured on pilot-scale. After initial characterization in coin half cells and by SEM, pouch full cells with fixed N/P ratios were built. Rate capability at different temperatures, and Post-Mortem analysis were carried out. Results from voltage relaxation, Li stripping, SEM measurements, glow discharge optical emission spectroscopy (GD-OES) depth profiling, and optical microscopy were validated against each other. A decreasing susceptibility to Li plating with increasing Si content in the anodes could be clearly observed. A critical C-rate was defined, at which Li plating was detected for the first time. It was also found that at 0 °C the critical C-rate increases with increasing Si contents. At 23 °C the SOC at which Li dendrites were first observed on the anode also increased with higher Si content.
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Zhang, Ji-Guang, Xia Cao, Phung M.-L. LE, Yan Jin, Ju-Myung Kim, and Wu Xu. "Development of Anode-Free Metal Batteries." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 36. http://dx.doi.org/10.1149/ma2022-01136mtgabs.
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Ever increasing need for electrical vehicles (EVs) continually pushes the boundary of high-density energy storage systems. To date, the state of the art of lithium (Li) ion batteries (LIBs) consisting of graphite anode and high voltage Li intercalation cathodes cannot satisfy the energy demand from these applications. By replacing graphite anode with Li metal anode (LMA), specific energy density of Li metal batteries (LMBs) can increase by more than 50% because LMA has a much higher specific capacity (3820 mAh g-1) than that of graphite (372 mAh g-1). To further increase the energy density of Li batteries, the concept of “anode-free” Li batteries (AFLBs) has been explored. Similar approach can also be used in “anode-free” sodium (Na) batteries (AFSBs) to further improve their energy densities. In this work, we will report our recent work on the development of AFLBs and AFSBs. The common challenges in these batteries will be analyzed and compared first. Several approaches, including development of novel electrolytes, substrate treatment, optimization of testing protocol and environment conditions, have been adopted to increase the cycle life of these batteries. At last, future perspective and application of anode-fee metal batteries will be discussed. References Niu, C.; Liu, D.; Lochala, J. A.; Anderson, C. S.; Cao, X.; Gross, M. E.; Xu, W.; Zhang, J.-G.; Whittingham, M. S.; Xiao, J.; Liu, J., Balancing interfacial reactions to achieve long cycle life in high-energy lithium metal batteries. Nature Energy 2021. Zhang, J.-G., Anode-less. Nature Energy 2019, 4 (8), 637-638. Pereira, N.; Amatucci, G. G.; Whittingham, M. S.; Hamlen, R., Lithium–titanium disulfide rechargeable cell performance after 35 years of storage. Journal of Power Sources 2015, 280, 18-22. Boyle, D. T.; Huang, W.; Wang, H.; Li, Y.; Chen, H.; Yu, Z.; Zhang, W.; Bao, Z.; Cui, Y., Corrosion of lithium metal anodes during calendar ageing and its microscopic origins. Nature Energy 2021.
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Greco, Eugenio, Giorgio Nava, Reza Fathi, Francesco Fumagalli, A. E. Del Rio-Castillo, Alberto Ansaldo, Simone Monaco, Francesco Bonaccorso, Vittorio Pellegrini, and F. Di Fonzo. "Few-layer graphene improves silicon performance in Li-ion battery anodes." Journal of Materials Chemistry A 5, no. 36 (2017): 19306–15. http://dx.doi.org/10.1039/c7ta05395a.
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A Li-ion battery anode based on few-layer graphene flakes and ultra-small Si nanoparticles shows a remarkable stability during cycling (0.04% capacity fading per cycle). Our approach offers a viable approach to develop new generation Li-ion battery anodes.
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Xie, Huanyu, Chaonan Wang, En Zhou, Hongchang Jin, and Hengxing Ji. "A black phosphorus-graphite hybrid as a Li-ion regulator enabling stable lithium deposition." JUSTC 52, no. 12 (2022): 3. http://dx.doi.org/10.52396/justc-2022-0105.
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Lithium (Li) metal anodes have been regarded as the most promising candidates for high energy density secondary lithium batteries due to their high specific capacity and low redox potential. However, the issues of Li dendrites caused by nonuniform lithium deposition during battery cycling severely hinder the practical applications of Li metal anodes. Herein, a hybrid of black phosphorus-graphite (BP-G) is introduced to serve as an artificial protective layer for the Li metal anode. The two-dimensional few-layer BP, which is lithophilic, combined with the high electronic conductive graphite can act as a regulator to adjust the migration of Li ions, delivering a uniform and stable lithium deposition. As the growth of lithium dendrites is inhibited, the utilization of Li metal achieves > 98.5% for over 500 cycles in Li||Cu half cells, and the life span is maintained over 2000 h in Li||Li symmetric cells with a low voltage hysteresis of 50 mV. Moreover, the LiFePO<sub>4</sub>||Li full cell with a BP-G Li-ion regulator presents significantly better specific capacity and cycling stability than that with the bare Li metal anode. Therefore, the introduction of the BP-G Li-ion regulator is demonstrated to be an effective approach to enable stable lithium deposition for rechargeable Li metal batteries.
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Shin, GeunHyeong, EunAe Cho, Hyeonmuk Kang, Taehee Kim, GyuSeong Hwang, and Junho Lee. "Metal Nitrate Embedded Polymeric Interlayer for Improving Cycling Stability of Li Metal Anode." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 262. http://dx.doi.org/10.1149/ma2022-012262mtgabs.
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Among secondary batteries using lithium, the use of lithium metal anodes for high capacity has become a hot topic. However, in lithium metal anodes, there is a major problem of dendritic growth and research are actively underway to address the issue. And it is reported that it is possible to improve the stability of Li metal anode by facilitating the movement of lithium ions through various additives to suppress dendritic growth and to make robust and stable SEI layer. To address the issue of dendritic growth of Li, using cesium nitrate is selected to improve the stability of the anode based on a mechanism by which a nitrogen-rich compounds lithiophilic to transport Li ion uniformly are formed in the SEI layer. And also the cesium element induces an cation electrostatic shielding effect while lithium metal is deposited and grown in the anode. In addition, since metal nitrates have very low solubility in carbonate-based electrolytes, polymer nanofiber-interlayer is synthesized by electrospinning to support metal nitrate and supply nitrate continuously and stably, while interlayer does not interfere with the movement of lithium ions through the nanofiber layer. In summary, a metal nitrate embedded polymer nanofiber layer is synthesized through an electrospinning method, then stabilization of a lithium surface and stability of a lithium metal anode are obtained by using an intermediate layer, and a relationship between an additive and SEI formation is identified at a limited solubility in carbonate electrolytes. The study result demonstrates that the lifetime of symmetric Li-Li cells and full cell with LCO cathodes improved greatly. And the deposition morphology of Li become dendrite-free and more uniform.
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Madani, Marzieh Sadat, Farrokh Roya Nikmaram, Azin Chitsazan, Farand Farzi, and Majid Monajjemi. "Cylindrical Capacitor-Anode Interaction Between Lithium Ion Batteries and (m, m)@(n, n) Double Wall Boron Nitride Nanotubes." Journal of Computational and Theoretical Nanoscience 13, no. 10 (October 1, 2016): 7293–302. http://dx.doi.org/10.1166/jctn.2016.5713.
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We report the stability and electronic structures of the double wall boron nitride nanotubes (DWBNNTs) due to interaction with anode lithium ion batteries (LIBs). Nano-Boron Nitride compounds have displayed great potential as anode materials for lithium ion batteries due to their unique structural, mechanical, and electrical properties. The measured reversible lithium ion capacities of SWBNTs//(Li)n//SWBNTs based anodes are considerably improved compared to the conventional graphite-based anodes. In this study (5, 5)@(7, 7) DWBNNTs, (5, 5)@(8, 8) DWBNNTs and (5, 5)@(9, 9) DWBNNTs have been localized inside the LIBs as an nano-capacitor to enhance electrochemical ratio of lithium ion capacities. Additionally, we have found the structure of (5, 5)@(8, 8) DWBNNTs can be to improve the capacity and electrical transport in anode-based LIBs. Therefore, the modification of cylindrical of BN and design of SWBNTs//(Li)n//SWBNTs structures provide strategies for improving the performance of material based anodes in LIBs. SWBNTs//(Li)n//SWBNTs could also be assembled into free-standing electrodes without any binder or current collector, which will lead to increased specific energy density for the overall battery design.
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Huang, Zhijia, Debin Kong, Yunbo Zhang, Yaqian Deng, Guangmin Zhou, Chen Zhang, Feiyu Kang, Wei Lv, and Quan-Hong Yang. "Vertical Graphenes Grown on a Flexible Graphite Paper as an All-Carbon Current Collector towards Stable Li Deposition." Research 2020 (July 11, 2020): 1–11. http://dx.doi.org/10.34133/2020/7163948.
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Lithium (Li) metal has been regarded as one of the most promising anode materials to meet the urgent requirements for the next-generation high-energy density batteries. However, the practical use of lithium metal anode is hindered by the uncontrolled growth of Li dendrites, resulting in poor cycling stability and severe safety issues. Herein, vertical graphene (VG) film grown on graphite paper (GP) as an all-carbon current collector was utilized to regulate the uniform Li nucleation and suppress the growth of dendrites. The high surface area VG grown on GP not only reduces the local current density to the uniform electric field but also allows fast ion transport to homogenize the ion gradients, thus regulating the Li deposition to suppress the dendrite growth. The Li deposition can be further guided with the lithiation reaction between graphite paper and Li metal, which helps to increase lithiophilicity and reduce the Li nucleation barrier as well as the overpotential. As a result, the VG film-based anode demonstrates a stable cycling performance at a current density higher than 5 mA cm-2 in half cells and a small hysteresis of 50 mV at 1 mA cm-2 in symmetric cells. This work provides an efficient strategy for the rational design of highly stable Li metal anodes.
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Ni, Jie, Yike Lei, Yongkang Han, Yingchuan Zhang, Cunman Zhang, Zhen Geng, and Qiangfeng Xiao. "Prefabrication of a Lithium Fluoride Interfacial Layer to Enable Dendrite-Free Lithium Deposition." Batteries 9, no. 5 (May 22, 2023): 283. http://dx.doi.org/10.3390/batteries9050283.
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Lithium metal is one of the most attractive anode materials for rechargeable batteries. However, its high reactivity with electrolytes, huge volume change, and dendrite growth upon charge or discharge lead to a low CE and the cycle instability of batteries. Due to the low surface diffusion resistance, LiF is conducive to guiding Li+ deposition rapidly and is an ideal component for the surface coating of lithium metal. In the current study, a fluorinated layer was prepared on a lithium metal anode surface by means of chemical vapor deposition (CVD). In the carbonate-based electrolyte, smooth Li deposits were observed for these LiF-coated lithium anodes after cycling, providing excellent electrochemical stability for the lithium metal anode in the liquid organic electrolyte. The CE of Li|Cu batteries increases from 83% for pristine Li to 92% for LiF-coated ones. Moreover, LiF-Li|LFP exhibits a decent rate and cycling performance. After 120 cycles, the capacity retention of 99% at 1C is obtained, and the specific capacity is maintained above 149 mAh/g. Our investigation provides a simple and low-cost method to improve the performance of rechargeable Li-metal batteries.
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Zhao, Lihong, Chaoshan Wu, Qing Ai, Liqun Guo, Zhaoyang Chen, Yanliang Liang, Jun Lou, Zheng Fan, and Yan Yao. "Operando Characterization of Plating and Stripping Dynamics of Li-Mg Alloy Anode and Sulfide Solid Electrolyte Interface." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 977. http://dx.doi.org/10.1149/ma2023-016977mtgabs.
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All-solid-state lithium metal batteries are projected to offer one of the highest specific energy among rechargeable batteries, positioning them as a front-runner for electric vehicle applications. Lithium metal anodes outperform conventional graphite anodes in terms of cell-level energy density. However, maintaining a conformal metal–electrolyte contact is a great challenge. The volumetric change of the lithium metal anode during stripping produces voids, which deteriorates the Li–electrolyte contact. To address this challenge, β-phase Li solid solution (i.e., Li-Mg alloy) has been shown to exhibit improved contact with the solid electrolyte during stripping. Moreover, Li solid solution has a similar electrochemical potential as Li, making it a potential replacement for Li metal anodes without sacrificing cell-level energy density. In this study, we show that the chemical properties of the alloy play an essential role in the morphological stability of metal–solid electrolyte interface. We compare the stripping behavior of pure Li and Li-Mg alloy anodes in argyrodite electrolyte and characterize the morphological evolution of the interface using operando scanning electron microscopy (SEM). We also analyze the electro-chemo-mechanical properties of Li and Li alloy anodes during stripping with galvanostatic electrochemical impedance spectroscopy (GEIS) to compare the influence of composition change and interfacial void on the electrode overpotential and interface resistance. Our research visualizes the morphological and compositional evolution of alloy metal anode during stripping and rationalizes their improved interfacial stability against solid electrolytes. Acknowledgment: This work was supported by the U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Vehicle Technologies Program under Contract DE-EE0008864. Figure 1
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Schulze, Maxwell C., Kae Fink, Jack Palmer, Mike Michael Carroll, Nikita Dutta, Christof Zweifel, Chaiwat Engtrakul, Sang-Don Han, Nathan R. Neale, and Bertrand J. Tremolet de Villers. "Reduced Electrolyte Reactivity of Pitch-Carbon Coated Si Nanoparticles for Li-Ion Battery Anodes." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 491. http://dx.doi.org/10.1149/ma2022-024491mtgabs.
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Silicon-based anodes for Li-ion batteries (LIB) have the potential to increase the energy density over graphite-based LIB anodes. However, silicon anodes exhibit poor cycle and calendar lifetimes due to mechanical instabilities and high chemical reactivity with the carbonate-based electrolytes that are typically used in LIBs. In this work, we synthesize a pitch-carbon coated silicon nanoparticle composite active material for LIB anodes that exhibits reduced chemical reactivity with the carbonate electrolyte compared to an uncoated silicon anode. Silicon primary particle sizes <10 nm minimize micro-scale mechanical degradation of the anode composite, while conformal coatings of pitch-carbon minimized the parasitic reactions between the silicon and the electrolyte. When matched with a high voltage NMC811 cathode, the pitch-carbon coated Si anode retains ~75% of its initial capacity over 1000 cycles. Efforts to increase the areal loading of the pitch-carbon coated silicon anodes to realize real energy density improvements over graphite anodes results in severe mechanical degradation on the electrode level. Developing procedures to engineer the architecture of the composite silicon anode may be a solution to this mechanical challenge. Figure 1
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Dzakpasu, Cyril Bubu, Myung-Hyun Ryou, and Yong Min Lee. "Effect of Carbon Nanotubes on the Electrochemical Performance of Li Powder Composite Anodes." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 427. http://dx.doi.org/10.1149/ma2022-024427mtgabs.
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To achieve the high energy density of lithium secondary batteries, the Li metal anode with a high theoretical capacity (3860 mAh g-1) and the lowest electrochemical potential (-3.04 vs. SHE) has attracted attention. However, Li metal is plagued with challenges such as irregular dendritic growth during cycling and low Coulombic efficiency (CE), which hinder its commercialization as an anode. Li metal powder (LMP) offers a solution to these problems by enlarging the surface area resulting in a lower effective current density. However, the commercial LMP passivated by Li2CO3 layer on the surface could hinder the electrical contact between individual LMPs as well as LMP and Cu current collector. Consequently, a series of LMP particle contact failures result in dead regions within the LMP electrode where the Li source cannot be fully activated. Herein, we report the effect of multiwalled CNTs on the electrochemical performance of Li metal powder-based anodes for Li metal batteries. The CNT-LMP anode exhibits a remarkable improvement in the electrochemical performance of coin cells compared to the bare LMP system. This improvement is attributed to the enhanced electrical connection between individual LMP particles, activation of full Li utilization, and the seeding effect of CNTs. Electrochemical properties were investigated using postmortem scanning electron microscopy and galvanostatic cycling techniques.
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Yan, Shuo, Mohamed Houache, Chae-Ho Yim, Ali Merati, Elena A. Baranova, Arnaud Weck, and Yaser Abu-Lebdeh. "Concentrated Electrolyte for Stable Lithium Metal Anode." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 551. http://dx.doi.org/10.1149/ma2023-012551mtgabs.
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Secondary lithium-ion batteries have been widely used as energy storage systems for portable electronics and electric vehicles. Instead of applying graphite as the anode, lithium (Li) metal has an ultrahigh theoretical capacity (3860 mAh/g) that could significantly increase battery’s energy density. Li dendrite formation is considered the main issue when using Li-metal anodes. Therefore, anode-free batteries are suggested as a solution to this obstacle. However, the major problem with anode-free batteries is their inferior cycling performance than reported lithium metal batteries, resulting from the formation of a fragile and fractured Solid-Electrolyte Interphase (SEI). To establish a robust SEI, novel lithium bis(trifluoromethylsulphonyl)imide (LiTFSI) and LiNO3-based electrolytes with four different ratios were prepared in the co-solvent system (1,3-dioxolane and 1,2-dimethoxyethane). Compared to the other three electrolytes, concentrated electrolyte (4M LiTFSI + 2 wt.% LiNO3 or 4+2) in Li||LiFePO4 cells indicated the highest initial discharge capacity of 154 mAh/g with a capacity retention of 78% after 50 cycles. Scanning electron microscopy was conducted to investigate the SEI morphology after the initial charge/discharge process. The deposited Li on the Li metal was highly dense, and no spiky or needle-like Li clusters were detected. Additionally, electrochemical impedance spectroscopy of the cells was measured after 1, 3, 5, and 10 cycles, respectively. The cells with 4+2 showed the smallest SEI resistance after different cycles, corresponding to a stable and less-resistive SEI formation.
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Wood, Marissa, Yiran Xiao, Megan C. Freyman, Cheng Zhu, Bo Wang, and Sichi Li. "Enabling Stable Li Metal Anodes for Solid-State Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 982. http://dx.doi.org/10.1149/ma2023-016982mtgabs.
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Solid-state batteries have the potential to transform energy storage by providing significantly higher energy densities and improved safety compared to conventional Li-ion batteries. However, robust high-capacity Li metal anodes are required to realize this technology. Current Li metal anode designs suffer from significant degradation over time due to non-uniform Li plating/stripping and loss of contact with the solid electrolyte during cycling. Carbon scaffold hosts have been shown to mitigate this problem in liquid electrolyte systems by creating a uniform electric field and providing abundant Li nucleation sites, but they have not been well explored in solid-state systems, which require the fabrication of more complicated mixed ion/electron conducting scaffolds to provide transport of both Li ions and electrons throughout the anode. We investigated the effect of scaffold architecture and chemistry on Li morphology and electrochemical performance using a combined experiment/theory approach. Scaffolds were characterized by SEM, Raman, and XPS before cycling in cells to evaluate their performance as hosts for Li plating/stripping. Atomistic and mesoscale modeling were used to help predict Li nucleation and current density hotspots and assist in guiding scaffold design. This work provides further insight into the relationship between anode design and Li metal cycling stability and will facilitate the development of safer, high-energy-density solid-state batteries. Lawrence Livermore National Laboratory is operated by Lawrence Livermore National Security, LLC, for the U.S. Department of Energy, National Nuclear Security Administration under Contract DE-AC52-07NA27344.
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Mondal, Abhishek N., Ryszard Wycisk, John Waugh, and Peter N. Pintauro. "Electrospun Si and Si/C Fiber Anodes for Li-Ion Batteries." Batteries 9, no. 12 (November 26, 2023): 569. http://dx.doi.org/10.3390/batteries9120569.
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Due to structural changes in silicon during lithiation/delithiation, most Li-ion battery anodes containing silicon show rapid gravimetric capacity fade upon charge/discharge cycling. Herein, we report on a new Si powder anode in the form of electrospun fibers with only poly(acrylic acid) (PAA) binder and no electrically conductive carbon. The performance of this anode was contrasted to a fiber mat composed of Si powder, PAA binder, and a small amount of carbon powder. Fiber mat electrodes were evaluated in half-cells with a Li metal counter/reference electrode. Without the addition of conductive carbon, a stable capacity of about 1500 mAh/g (normalized to the total weight of the anode) was obtained at 1C for 50 charge/discharge cycles when the areal loading of silicon was 0.30 mgSi/cm2, whereas a capacity of 800 mAh/g was obtained when the Si loading was increased to ~1.0 mgSi/cm2. On a Si weight basis, these capacities correspond to >3500 mAh/gSi. The capacities were significantly higher than those found with a slurry-cast powdered Si anode with PAA binder. There was no change in fiber anode performance (gravimetric capacity and constant capacity with cycling) when a small amount of electrically conductive carbon was added to the electrospun fiber anodes when the Si loading was ≤1.0 mgSi/cm2.
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Lou, Ding, Haiping Hong, Marius Ellingsen, and Rob Hrabe. "Supersonic cold-sprayed Si composite alloy as anode for Li-ion batteries." Applied Physics Letters 122, no. 2 (January 9, 2023): 023901. http://dx.doi.org/10.1063/5.0135408.
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The increasing demand for lithium-ion batteries (LIBs) continuously stimulates the research community to seek advanced fabrication of anodes with improved performance and lifespan. Silicon (Si), as one of the most promising anode materials, has been the main focus of both research and industry. In this paper, we report a type of Si alloy anode for LIBs manufactured by the supersonic cold spray technique. The microscopic analysis revealed the uniform morphologies of the anodes, indicating that Si and other metal particles were well bonded. Specific discharge capacities were obtained for the cold-sprayed anodes by half-coin cell tests, with the highest value of 1047 mAh g−1 at a current rate of 0.05 C. Most importantly, the energy-dispersive x-ray spectroscopy results demonstrated none oxidation of the powders after the cold spray process. The results strongly indicate that the concept of using cold spray technique to fabricate Si alloy anode is feasible. Compared to the conventional methods of fabricating Si anodes, the cold spray approach is simple, convenient, and scalable. This method may revolutionarily change the LIBs industries.
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Sharma, Subash, Tetsuya Osugi, Sahar Elnobi, Shinsuke Ozeki, Balaram Paudel Jaisi, Golap Kalita, Claudio Capiglia, and Masaki Tanemura. "Synthesis and Characterization of Li-C Nanocomposite for Easy and Safe Handling." Nanomaterials 10, no. 8 (July 29, 2020): 1483. http://dx.doi.org/10.3390/nano10081483.
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Metallic lithium (Li) anode batteries have attracted considerable attention due to their high energy density value. However, metallic Li is highly reactive and flammable, which makes Li anode batteries difficult to develop. In this work, for the first time, we report the synthesis of metallic Li-embedded carbon nanocomposites for easy and safe handling by a scalable ion beam-based method. We found that vertically standing conical Li-C nanocomposite (Li-C NC), sometimes with a nanofiber on top, can be grown on a graphite foil commonly used for the anodes of lithium-ion batteries. Metallic Li embedded inside the carbon matrix was found to be highly stable under ambient conditions, making transmission electron microscopy (TEM) characterization possible without any sophisticated inert gas-based sample fabrication apparatus. The developed ion beam-based fabrication technique was also extendable to the synthesis of stable Li-C NC films under ambient conditions. In fact, no significant loss of crystallinity or change in morphology of the Li-C film was observed when subjected to heating at 300 °C for 10 min. Thus, these ion-induced Li-C nanocomposites are concluded to be interesting as electrode materials for future Li-air batteries.
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Thangadurai, Venkataraman. "High-Performance Lithium Metal Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 652. http://dx.doi.org/10.1149/ma2023-024652mtgabs.
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The success of rechargeable lithium-ion batteries (LIBs) has brought evident convenience to human society, but state-of-the-art LIBs with a graphite anode are approaching their energy density limits. Li metal is considered the ultimate anode material due to its ultra-high theoretical specific capacity of 3860 mAh g-1, which is more than 10 times higher than lithiated graphite. Nonetheless, Li metal anode suffers from poor safety and low cycling efficiency due to its high reactivity. Electrolytes that work with Li anode should possess excellent stability against Li metal or form a highly passivating interface. It is also critical to control the amount of Li in the cell, preferably having no excess Li at the anode side. In this talk next-generation solid state and hybrid electrolytes based on Li-stuffed garnets that enable high-performance Li metal batteries will be discussed.
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Chen, Jie, Bin He, Zexiao Cheng, Zhixiang Rao, Danqi He, Dezhong Liu, Xiang Li, Lixia Yuan, Yunhui Huang, and Zhen Li. "Reactivating Dead Li by Shuttle Effect for High-Performance Anode-Free Li Metal Batteries." Journal of The Electrochemical Society 168, no. 12 (December 1, 2021): 120535. http://dx.doi.org/10.1149/1945-7111/ac42a5.
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Anode-free Li metal batteries are considered the ultimate configuration for next-generation high energy-density Li-based batteries due to the elimination of excess Li metal. However, the limited Li source aggravates issues such as dendrite growth and “dead” Li formation. Any Li loss caused by the SEI formation and dead Li has a great influence on the performance of the full cell. Here, we introduce LiI with shuttle effect to suppress the Li dendrites and reactivate the dead Li in the anode-free LiFePO4 (LFP) ∣Cu full cells. During cycling, the iodine transforms between I− and I3 −, and a chemical reactions occur spontaneously between I3 − and Li dendrites or dead Li. The generated Li+ in the electrolyte remains active in the following cycling. The anode-free LFP∣Cu cells deliver an initial discharge capacity of 139 mAh g−1 and maintain capacities of 100 mAh g−1 with a capacity retention of 72% after 100 cycles. Both the anode-free LFP∣Cu coin cells and pouch cells with LiI additive show much-improved performances. This work provides a new strategy for high-performance anode-free Li metal batteries.
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Delaporte, Nicolas, Alexis Perea, Steve Collin-Martin, Mireille Léonard, Julie Matton, Vincent Gariépy, Hendrix Demers, Daniel Clément, Etienne Rivard, and Ashok Vijh. "Li Metal Anode with a LiZn Alloy Interlayer for Li-Metal Polymer Batteries." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 970. http://dx.doi.org/10.1149/ma2023-016970mtgabs.
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All-solid-state batteries (ASSB) require stable and safe Li metal anode, which needs surface preparation to increase lithium diffusion and impede the formation of dendrites. In this work, the formation of a thin LiZn layer on lithium metal using sputter deposition is reported. This method was selected due to the absence of solvents and by-products generated during the modification, for its rapidity and because the formation of the alloy is performed in a clean and controlled atmosphere. Zinc has been chosen for its low cost and high Li+ ion diffusion coefficient of the corresponding LiZn alloy that is 1000 times higher than lithium. Different parameters for the Zn deposition were investigated such as the distance between the Zn target and Li foil, the effect of substrate tilt and the direct current applied to the target. Electrochemical performance of LiFePO4/solid polymer electrolyte/Li ASSB demonstrated the superiority of the LiZn anodes and the clear influence of deposition parameters on the durability and performance at high C-rates. Scanning electron microscopy images of the cross-sectional view of LFP/SPE/Li stackings extracted from pouch cells after cycling showed an evident migration of Zn into the bulk Li metal anode as well as the formation of AlZn nanoparticles. In addition, the formation of Li dendrites was effectively reduced for the cells made with the LiZn-protected Li metal anode. Finally, we reported an interesting observation concerning the influence of sputter conditions on the variation of morphology of Li grains.
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Rodrigues, Marco-Tulio F. "(Invited) The Reservoir Effect: When Capacity Measurements Cannot Track Cell Aging." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 553. http://dx.doi.org/10.1149/ma2023-012553mtgabs.
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The initial capacity that is provided by a Li-ion battery is limited by the amount of Li+ that is supplied by the cathode. During the life of a cell, growth of the solid electrolyte interphase (SEI) will slowly consume Li+, which generally leads to capacity fade. Capacity and coulombic efficiency measurements are commonly used in battery research to quantify the evolution of SEI growth. In this talk, we show that, in reality, such measurements can often be unreliable sources of information about the extent of aging endured by the cell.[1,2] A core problem with relying on capacity measurements to track aging is that they may not probe all the Li+ that is present in the cell. See for example Figure 1a, which shows the voltage profiles of three types of anodes (graphite, silicon-graphite and SiOx) during the discharge of a full-cell. At the end of discharge, we assume that all anodes will experience a same potential of 0.6 V vs Li/Li+, which is the point in which the profiles intersect in the figure. Portions of the voltage profiles to the right of this point of intersection indicate Li+ that will remain in the anode even after the cell is “fully” discharged. That is, Li+ that was inserted into the anode during the initial charge, but that cannot be recovered at the voltage cutoff selected for cell discharge. The magnitude of this “reservoir” of Li+ depends on the shape of the voltage profile of the anode at high potentials. Failure to account for the existence of this reservoir will, for example, distort estimates about the initial Li+ consumption to form the SEI. To make matters worse, capacity stored in this Li+ reservoir can slowly be accessed as the cell ages, blurring the correlation between capacity measurements and SEI growth. During cell charging, most cathode materials of commercial interest will experience an increase in potential as they delithiate (Figure 1b). If some of that Li+ is consumed at the SEI, then the cathode cannot be restored to its original state of lithiation once the cell is fully discharged. In other words, aging will cause the cathode to experience increasing potentials once the cell meets the discharge cutoff voltage. Assuming that voltage cutoffs are constant for all cycles, an increase in cathode potential by ΔU would prompt an equal increase in the potential of the anode. A key consequence is that this bump in potential will lead to partial delithiation of the Li+ reservoir stored in the anode, releasing “extra” Li+ that can go back into the cathode. Accessing this extra capacity will offset some of the measurable Li+ losses to the SEI. Since the size of this reservoir is larger in Si than in graphite, capacity measurements in silicon cells can largely underestimate the true extent of SEI growth, and may conceal relatively high levels of cell aging under the appearance of satisfactory cycling performance. The example above shows that the reliability of using capacity measurements for conveying information about aging depends on the anode used in the cell. This same general behavior can also arise when comparing different cathode materials, or even different operating conditions (such as cycling rate and depth of discharge) for a same type of battery. This talk will discuss some of these cases, and how they can affect the diagnostic of aging in Li-ion cells. Figure 1. a) Assumed voltage profiles for anodes during the discharge of hypothetical full-cells. At the discharge cutoff voltage, all anodes will initially experience a typical value of ~0.6 V vs. Li/Li+ (indicated by the intersection point). Regions to the right of that point indicate capacity that remains stored at the anode even when the full-cell is nominally fully discharged. b) Example of successive charge and discharge half-cycles in a NMC811 cathode. The solid black line indicates portions of the voltage profile that are actively utilized in the cathode. When Li+ is lost to the SEI, the cathode cannot be restored to the Li+ content it exhibited at the beginning of charge, leading to an increase in cathode potential when the full-cell reaches the cutoff voltage. References [1] Rodrigues, J. Electrochem Soc. 169, 080524 (2022) [2] Rodrigues, J. Electrochem Soc. 169, 110514 (2022) Acknowledgments: This research was supported by the U.S. Department of Energy’s Vehicle Technologies Office under the Silicon Consortium Project, directed by Brian Cunningham, and managed by Anthony Burrell. Figure 1
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Kang, Dongyoon, Cyril Bubu Bubu Dzakpasu, Sun-Yul Ryou, Hongkyung Lee, and Yong Min Lee. "Formation of N-Rich Solid Electrolyte Interphase with LiNO3 Solution for Lithium Metal Powder Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 763. http://dx.doi.org/10.1149/ma2023-024763mtgabs.
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Conventional manufacturing process of Li metal anodes employs extrusion-pressing or deposition methods resulting in sheet or film-types, respectively. Considering the demands for high-gravimetric energy density, thinner Li metal is crucial for realizing the desired weight ratio of anode in Li metal batteries (LMBs). However, during the manufacturing process at high rate, there could be limitations such as Li damage or dendritic growth caused by excessive pressure or non-uniform deposition. Li metal powders (LMPs) are beneficial for fabricating thin Li anodes within a short time via a slurry coating process. Despite the advantages of LMP, the Li2CO3 passivation layer unevenly covering the LMP surface results in dendritic Li growth. Thus, modification of the passivation layer is very crucial to control the Li plating/stripping behavior. Here, we suggest a LiNO3 solution-treated LMP electrode for securing robust cyclability with low overpotential in LMBs. The dissolved LiNO3 in the LMP slurry can effectively modify the passivation layer into an N-rich SEI, enabling a uniform Li+ flux. Additionally, the well-distributed LiNO3 in the LMP anode could continuously repair the SEI during cycling via a slow-release mechanism into the carbonate-based electrolyte system. As a result, the LiNO3-treated LMP electrode effectively enhances the performance and stability of LMBs. Therefore, LiNO3 solution treatment of Li metal is an attractive approach to achieving a stable and robust SEI in LMBs.
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Chae, Somin, Hyung-kyu Lim, and Sangheon Lee. "Computation-Based Investigation of Motion and Dynamics of Lithium in Phase Separated Silicon-Oxide Anode Materials." ECS Meeting Abstracts MA2022-01, no. 55 (July 7, 2022): 2269. http://dx.doi.org/10.1149/ma2022-01552269mtgabs.
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Si attracts significant attention as an alternative anode material to replace the conventional graphite anode in lithium-ion batteries (LIBs). Si offers extremely high theoretical energy-storage capacity of 4200 mAh/g for Li4.4Si, while the theoretical energy-storage capacity of graphite is only 372 mAh/g for Li/C6. In addition, Si is abundant, eco-friendly, and non-toxic, and it also has a safe thermodynamic potential with an average voltage of about 0.4 V vs. Li+/Li, making them attractive candidates for LIB anodes. However, the capacity of the Si anode exhibits a relatively high initial charge capacity and then rapidly decreases as the charge/discharge cycle proceeds, hampering its extensive application. This rapid performance degradation can be attributed to the poor connection between the active material and the current collector resulting from the severe volume expansion and contraction of the Si particles during the repeated charge and discharge cycles, respectively. Controlled addition of O to Si is often taken as a viable approach to utilize Si as an anode material. Silicon suboxides (SiOx, 0 < x < 2), compared with Si, offer a low energy capacity but a high stability against volume expansion. As a result, silicon monoxide (SiO) anodes are indeed commercialized by being blended with graphite. However, only low amounts (about 5 wt%) of SiO are blended with graphite because of the poor first cycle efficiency of SiO. During the charge process, SiOx reacts with Li and produces in-situ byproducts such as Li2O and Li-silicates, which are irreversible in following discharge cycles. This irreversible Li consumption is known to decrease the initial Coulombic efficiency (ICE) of SiO, typically below 75%. The low ICE of SiOx along with its inherently poor electronic conductivity leads to poor rate performance and increased capacity decay, hindering its substantial application in LIBs. To realize more extensive application of SiOx for LIB anodes, physical properties of SiOx should be improved in a direction to mitigate the low ICE issue. In this study, we investigate the motion and dynamics of a Li atom in SiOx by performing a series of first principles-based atomistic simulations. To this end, we perform Monte Carlo simulations within a continuous random network model to generate realistic SiOx structures with varying O-to-Si ratios. Then, we implement a density-functional theory calculation-based path sampling scheme to obtain detailed thermodynamic information when a Li atom penetrates a SiO matrix. Subsequent electronic structure analysis reveals that the thermodynamic stability of a Li atom is determined by local Si-O network environment surrounding Li. The identified thermodynamic information regarding the Li dynamics in SiO provides additional insight into the origin and solutions of the low ICE, highlighting the importance of controlling the SiO morphology during the synthesis of SiO. This fundamental understanding can be an important theoretical basis for developing practically applicable high-ICE silicon suboxide-based anode materials. Figure 1
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Dasari, Harika, and Eric Eisenbraun. "Predicting Capacity Fade in Silicon Anode-Based Li-Ion Batteries." Energies 14, no. 5 (March 6, 2021): 1448. http://dx.doi.org/10.3390/en14051448.
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While silicon anodes hold promise for use in lithium-ion batteries owing to their very high theoretical storage capacity and relatively low discharge potential, they possess a major problem related to their large volume expansion that occurs with battery aging. The resulting stress and strain can lead to mechanical separation of the anode from the current collector and an unstable solid electrolyte interphase (SEI), resulting in capacity fade. Since capacity loss is in part dependent on the cell materials, two different electrodes, Lithium Nickel Oxide or LiNi0.8Co0.15Al0.05O2 (NCA) and LiNi1/3Mn1/3Co1/3O2 (NMC 111), were used in combination with silicon to study capacity fade effects using simulations in COMSOL version 5.5. The results of these studies provide insight into the effects of anode particle size and electrolyte volume fraction on the behavior of silicon anode-based batteries with different positive electrodes. It was observed that the performance of a porous matrix of solid active particles of silicon anode could be improved when the active particles were 150 nm or smaller. The range of optimized values of volume fraction of the electrolyte in the silicon anode were determined to be between 0.55 and 0.40. The silicon anode behaved differently in terms of cell time with NCA and NMC. However, NMC111 gave a high relative capacity in comparison to NCA and proved to be a better working electrode for the proposed silicon anode structure.
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Sacci, Robert L., Andrew S. Westover, Zhiao Yu, and Zhenan Bao. "Dynamic Impedance Spectroscopy of Lithium Plating from Next Generation Electrolytes." ECS Meeting Abstracts MA2022-02, no. 2 (October 9, 2022): 149. http://dx.doi.org/10.1149/ma2022-022149mtgabs.
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The anode-free cells have emerged due to the need to maximize Li metal batteries' energy density. However, anode-free Li batteries suffer from short cycle life because of the lack of Li inventory at the anode. Freshly deposited Li metal anodes usually take hundreds of cycles to reach initial SEI stabilization optimum coulombic efficiency (CE) due to initial SEI stabilization and electrode activation. The anode-free cell design requires high Li metal CE over the whole cycling life, particularly during the initial activation cycles. A holistic approach to electrolyte design, mechanism understanding, and battery engineering is needed to fulfill these requirements. Here, we present a mechanistic study on lithium plating and stripping from next generation electrolytes. We conducted dynamic impedance spectroscopy (dEIS) to probe the formation and evolution of the SEI during Li plating and stripping on copper current collectors. dEIS superimposes a multisine waveform atop the dc stimulus signal, as shown by the lightly shaded curves in Fig 1 (top left). We applied a sliding window FFT protocol that takes the complex ratio of the measured potential and current signals obtained from Fig 1 (top right) and transforms it into complex impedance. We will discuss two Li platting systems, Lipon (an amorphous ceramic) and a liquid electrolyte with stabilizing additives. We observed drastic changes in the cells' impedance during plating and stripping, Figure 1 (bottom plots). We will show how the passivation layer's impedance continues to evolve during Li cycling and accounts for a significant amount of the overall cell resistance. The US Department of Energy’s Energy Efficiency and Renewable Energy Vehicles Technologies Office provided funding for this work under the US-German Cooperation on Energy Storage: Lithium-Solid-Electrolyte Interfaces program. Figure 1
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Liu, Qingsong, Yue Wang, Jian Zhang, Jianquan Liang, Shuaifeng Lou, Ge Zhu, Hanwen An, et al. "Effective electron–ion percolation network enabled by in situ lithiation for dendrite-free Li metal battery." Applied Physics Letters 121, no. 15 (October 10, 2022): 153901. http://dx.doi.org/10.1063/5.0108998.
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The development of a lithium metal anode has been hindered by the problem of lithium dendrites. The fast and homogeneous ion transport to achieve even lithium plating is challenging but still remains elusive. Improving the single conduction of ions or electrons is not enough to achieve dendrite-free and long life Li–metal composite electrodes. Herein, we use in situ lithiation and electroplating methods to construct an effective mixed electron–ion percolation network composite anode. The mixed ion–electron conductive framework can build a stable interface that provides nucleation sites for Li plating. At the same time, the 3D percolation network composed of 3D nanosheets can facilitate the fast transport of ions and electrons, enabling uniform lithium plating inside the skeleton. As a result, the composite anodes exhibit a stable dendrite-free Li stripping/plating process with low overpotential. Furthermore, the full cell using the composite anode coupled with the LiFePO4 cathode displays high cycle stability with a capacity retention rate of about 100% after 500 cycles. The present strategy of the mixed ion–electron conductive skeleton could further promote the development of the next-generation lithium metal anode.
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Dong, Rui Zhi. "Comparative Studies on VS2 Bilayer and VS2/Graphene Heterostructure as the Anodes of Li Ion Battery." Key Engineering Materials 894 (July 27, 2021): 61–66. http://dx.doi.org/10.4028/www.scientific.net/kem.894.61.
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Due to the development of various mobile electronic devices, such as electric vehicles, rechargeable ion batteries are becoming more and more important. However, the current commercial lithium-ion batteries have obvious defects, including poor safety from Li dendrite and flammable electrolyte, quick capacity loss and low charging and discharging rate. It is very important to find a better two-dimensional material as the anode of the battery to recover the disadvantages. In this paper, first principles calculations are used to explore the performances of VS2 bilayer and VS2 / graphene heterostructure as the anodes of Li ion batteries. Based on the calculation of the valences, binding energy, intercalation voltage, charge transfer and diffusion barrier of Li, it is found that the latter can be used as a better anode material from the perspective of insertion voltage and binding energy. At the same time, the former one is better in terms of diffusion barrier. Our study provides a comprehensive understanding on VS2 based 2D anodes.
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Li, Yao Yao, Yin Hu, and Cheng Tao Yang. "Regulating Li<sup>+</sup> Transfer and Solvation Structure via Metal-Organic Framework for Stable Li Anode." Key Engineering Materials 939 (January 25, 2023): 123–27. http://dx.doi.org/10.4028/p-in7u78.
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Lithium metal batteries (LMBs) possess large application potential for advanced rechargeable batteries due to the high energy density (> 500 Wh kg−1) and alternative cathode materials. Random Li dendrite growth caused by uneven Li+ distribution and local ion depletion near surface of Li anode induces battery failure with inferior long-term stability. Therefore, regulation of ion distribution near anode surface is essential to realize dendrite-free and uniform Li deposition. Herein, a metal-organic framework (MOF), i.e., ZIF-8, is applied to regulate Li+ solvation structure via unsaturated metal-ion sites to achieve uniform Li+ distribution and Li deposition. A stable cycling performance over 800 h for Li symmetrical cell at 3 mA cm−2 and 3 mAh cm−2 without short circuit is realized. The facilitated Li+ solvation via the adsorption effect of metal-ion sites on anions is demonstrated, which further enhances the uniform Li+ distribution near Li anode surface. This work demonstrates an effective strategy for regulating ion coordination and Li+ distribution to stabilize Li anode via MOF-based materials.
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Meng, Shirley, Wurigumula Bao, and Bingyu Lu. "(Keynote) Parameterize Important Factors for Li Metal Batteries: Cycle Life, Calendar Life and Reactivity." ECS Meeting Abstracts MA2023-01, no. 56 (August 28, 2023): 2731. http://dx.doi.org/10.1149/ma2023-01562731mtgabs.
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The lithium (Li) metal anode is essential for next-generation high-energy-density lithium metal batteries. The calendar life and reactivity (safety) are equally important to cycle stability for the real application of Li metal anode in different devices. Our recent studies have identified that preventing Li dendrite growth by stacking pressure could improve cycle life by consuming less electrolyte and preventing inactive Li0 accumulation. A similar conclusion is obtained in the study of electrodepositing Li metal anode calendar life and reactivity (safety), in which the porosity of the deposited Li dominates the Li metal corrosion rate and reactivity. The larger the porosity of deposited Li, the faster the corrosion rate/higher reactivity will be. Moreover, all cell components must be considered when it comes to the reactivity (safety) of Li metal batteries because components may react with each other. Our results revealed that dense Li metal anode owns similar reactivity as lithiated graphite/ Li-Si alloy. All results facilitate lithium metal battery design and manufacturing.