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1
Han, Renwu. "Si nanomaterials in lithium-ion battery anode." Applied and Computational Engineering 26, no. 1 (November 7, 2023): 62–72. http://dx.doi.org/10.54254/2755-2721/26/ojs/20230797.
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Due to its high specific capacity, silicon anode has gained interest on a global scale as the anode of next-generation lithium-ion batteries (LIBs). However, it is challenging for silicon anodes to replace graphite anodes for widespread use due to the inevitable volume expansion and SEI film development generated by silicon during the lithiation/delithiation process. Among these, the advancement of nanotechnology has sped up the development of silicon anodes. This paper reviews nanotechnology applied in the Si anode to improve the battery performance. The volume expansion of Si is effectively decreased by reducing the volume of the silicon anode in order to increase its specific surface area. Additionally, the smaller negative electrode reduces the distance traveled by lithium ions, greatly increasing the silicon negative electrode's efficiency. At present, the main silicon nano-anode materials include nanoparticles, nanowires, nanosheets, nanotubes, nanoporous materials and so on. It is hoped that this review will provide a deep prospect introduction to the nano-silicon anode. Pure silicon nanoparticles and silicon nanowires, and new nanomaterials composed of them with graphite, graphene, metals, etc.
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Han, Renwu. "Si nanomaterials in lithium-ion battery anode." Applied and Computational Engineering 26, no. 1 (November 7, 2023): 62–72. http://dx.doi.org/10.54254/2755-2721/26/20230797.
Full textAbstract:
Due to its high specific capacity, silicon anode has gained interest on a global scale as the anode of next-generation lithium-ion batteries (LIBs). However, it is challenging for silicon anodes to replace graphite anodes for widespread use due to the inevitable volume expansion and SEI film development generated by silicon during the lithiation/delithiation process. Among these, the advancement of nanotechnology has sped up the development of silicon anodes. This paper reviews nanotechnology applied in the Si anode to improve the battery performance. The volume expansion of Si is effectively decreased by reducing the volume of the silicon anode in order to increase its specific surface area. Additionally, the smaller negative electrode reduces the distance traveled by lithium ions, greatly increasing the silicon negative electrode's efficiency. At present, the main silicon nano-anode materials include nanoparticles, nanowires, nanosheets, nanotubes, nanoporous materials and so on. It is hoped that this review will provide a deep prospect introduction to the nano-silicon anode. Pure silicon nanoparticles and silicon nanowires, and new nanomaterials composed of them with graphite, graphene, metals, etc.
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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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Cao, Xia, Qiuyan Li, Ran Yi, Wu Xu, and Ji-Guang Zhang. "Stabilization of Silicon Anode By Advanced Localized High Concentration Electrolytes." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 247. http://dx.doi.org/10.1149/ma2022-023247mtgabs.
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The rapid market penetration of EVs requires batteries with higher energy densities. However, graphite-based lithium-ion batteries (LIBs) has eventually reached their practical limit and an anode with higher specific capacities is required to further improve energy density of LIBs. In this regard, silicon (Si) anode has been pursued as one of the most promising anodes because it exhibits a capacity ten times as high as those of graphite. However, fast capacity fade during cycling and calendar aging limits the practical application of Si-based anodes due to its severe volume changes and continuous side reactions with electrolyte. Therefore, development of electrolytes that are stable with an electrode with large volume expansion is critical to stabilize the Si anode and enable the full potential of the Si based LIBs. In the case of graphite, a stable solid electrolyte interphase (SEI) can be formed on graphite surface because it does not experience large volume change (< 10%), so the SEI can prevent further reactions between graphite and electrolyte once it is formed. In contrast, the SEI layer formed on Si anode must be mechanically strong and withhold large volume changes (>300%). This work reports the design and performance of advanced localized high concentration electrolytes (LHCEs) for Si anode, in which robust SEI forms on the surface of Si anode and protects the Si anode from the pulverization caused by the large volume changes. As a result, the overall performance of the Si based LIBs are greatly improved by using the optimized LHCEs. The electrolytes have been tailored for different applications, including high voltage (4.45 V), high temperature (45°C) and high rate (> 2C) applications. The fundamental understandings of LHCEs and corresponding SEIs developed in this work can guide the design of new electrolytes for other anodes with large volume expansion.
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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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Durmus, Yasin Emre, Christoph Roitzheim, Hermann Tempel, Florian Hausen, Yair Ein-Eli, Hans Kungl, and Rüdiger-A. Eichel. "Analysis on discharge behavior and performance of As- and B-doped silicon anodes in non-aqueous Si–air batteries under pulsed discharge operation." Journal of Applied Electrochemistry 50, no. 1 (December 2, 2019): 93–109. http://dx.doi.org/10.1007/s10800-019-01372-5.
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Abstract Very high theoretical specific energies and abundant resource availability have emerged interest in primary Si–air batteries during the last decade. When operated with highly doped Si anodes and EMIm(HF)2.3F ionic liquid electrolyte, specific energies up to 1660 Wh kgSi−1 can be realized. Owing to their high-discharge voltage, the most investigated anode materials are $$\langle 100\rangle$$⟨100⟩ oriented highly As-doped Si wafers. As there is substantial OCV corrosion for these anodes, the most favorable mode of operation is continuous discharge. The objective of the present work is, therefore, to investigate the discharge behavior of cells with $$\langle 100\rangle$$⟨100⟩ As-doped Si anodes and to compare their performance to cells with $$\langle 100\rangle$$⟨100⟩ B-doped Si anodes under pulsed discharge conditions with current densities of 0.1 and 0.3 mA cm−2. Nine cells for both anode materials were operated for 200 h each, whereby current pulse time related to total operating time ranging from zero (OCV) to one (continuous discharge), are considered. The corrosion and discharge behavior of the cells were analyzed and anode surface morphologies after discharge were characterized. The performance is evaluated in terms of specific energy, specific capacity, and anode mass conversion efficiency. While for high-current pulse time fractions, the specific energies are higher for cells with As-doped Si anodes, along with low-current pulse fractions the cells with B-doped Si anodes are more favorable. It is demonstrated, that calculations for the specific energy under pulsed discharge conditions based on only two measurements—the OCV and the continuous discharge—match very well with the experimental data. Graphic abstract
7
Liu, Xiaoxian, Juan Liu, Xiaoyu Zhao, Dianhong Chai, Nengwen Ding, Qian Zhang, and Xiaocheng Li. "Turning Complexity into Simplicity: In Situ Synthesis of High-Performance Si@C Anode in Battery Manufacturing Process by Partially Carbonizing the Slurry of Si Nanoparticles and Dual Polymers." Molecules 29, no. 1 (December 28, 2023): 175. http://dx.doi.org/10.3390/molecules29010175.
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For Si/C anodes, achieving excellent performance with a simple fabrication process is still an ongoing challenge. Herein, we report a green, facile and scalable approach for the in situ synthesis of Si@C anodes during the electrode manufacturing process by partially carbonizing Si nanoparticles (Si NPs) and dual polymers at a relatively low temperature. Due to the proper mass ratio of the two polymer precursors and proper carbonization temperature, the resultant Si-based anode demonstrates a typical Si@C core–shell structure and has strong mechanical properties with the aid of dual-interfacial bonding between the Si NPs core and carbon shell layer, as well as between the C matrix and the underlying Cu foil. Consequently, the resultant Si@C anode shows a high specific capacity (3458.1 mAh g−1 at 0.2 A g−1), good rate capability (1039 mAh g−1 at 4 A g−1) and excellent cyclability (77.94% of capacity retention at a high current density of 1 A g−1 after 200 cycles). More importantly, the synthesis of the Si@C anode is integrated in situ into the electrode manufacturing process and, thus, significantly decreases the cost of the lithium-ion battery but without sacrificing the electrochemical performance of the Si@C anode. Our results provide a new strategy for designing next-generation, high-capacity and cost-effective batteries.
8
Wang, Jingbo, Li Cao, Songyuan Li, Jiejie Xu, Rongshi Xiao, and Ting Huang. "Effect of Laser-Textured Cu Foil with Deep Ablation on Si Anode Performance in Li-Ion Batteries." Nanomaterials 13, no. 18 (September 11, 2023): 2534. http://dx.doi.org/10.3390/nano13182534.
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Si is a highly promising anode material due to its superior theoretical capacity of up to 3579 mAh/g. However, it is worth noting that Si anodes experience significant volume expansion (>300%) during charging and discharging. Due to the weak adhesion between the anode coating and the smooth Cu foil current collector, the volume-expanded Si anode easily peels off, thus damaging anode cycling performance. In the present study, a femtosecond laser with a wavelength of 515 nm is used to texture Cu foils with a hierarchical microstructure and nanostructure. The peeling and cracking phenomenon in the Si anode are successfully reduced, demonstrating that volume expansion is effectively mitigated, which is attributed to the high specific surface area of the nanostructure and the protection of the deep-ablated microgrooves. Moreover, the hierarchical structure reduces interfacial resistance to promote electron transfer. The Si anode achieves improved cycling stability and rate capability, and the influence of structural features on the aforementioned performance is studied. The Si anode on the 20 μm-thick Cu current collector with a groove density of 75% and a depth of 15 μm exhibits a capacity of 1182 mAh/g after 300 cycles at 1 C and shows a high-rate capacity of 684 mAh/g at 3 C.
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Kumar, Kuldeep, Ian L. Matts, Andrei Klementov, Scott Sisco, Dennis A. Simpson, Edward R. Millero, Kareem Kaleem, Gina M. Terrago, and Se Ryeon Lee. "Improving Fundamental Understanding of Si-Based Anodes Using Carboxymethyl Cellulose (CMC) and Styrene-Butadiene Rubber (SBR) Binder for High Energy Lithium Ion Battery Applications." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 420. http://dx.doi.org/10.1149/ma2022-012420mtgabs.
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With increasing demand of high energy density lithium ion batteries, silicon (Si) based anodes are an obvious substitute of graphite based systems due to their high capacity. However, large volume changes of Si during lithiation and delithiation processes causes pulverization of silicon particles. The resulting reduction in electrical continuity and solid electrolyte interphase (SEI) growth within the anode leads to a fast depletion of lithium reservoirs and an accelerates battery failure. High energy lithium ion battery applications such as electrical vehicles and electronic devices require high capacity retention over extended cycling, so improving performance of Si-based anodes is a critical need for many applications. Commonly, a combination of sodium carboxymethyl cellulose (CMC) and styrene-butadiene rubber (SBR) is used as a binder for waterborne Si anode slurries. In these systems, carboxyl (-COOH) groups on CMC form chemical bonding with hydroxyl (-OH) groups on Si active material surface and SBR addition provides enhanced flexibility in the anode layer. Several reports on electrode integrity improvement through adhesion promoters, increased crosslinking, different binding groups, etc. are available in the literature. Delving deeper into the weak mechanical integrity of Si based anodes, and understanding the parameters influencing the fabrication process and subsequent properties, is important. This presentation will focus on several variations in Si based anode slurries and electrodes using CMC-SBR binders. Physical, mechanical, and electrochemical properties are extensively studied as a function of these parameters and will be discussed.
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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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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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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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Karki, Peshal, Morteza Sabet, Apparao M. Rao, and Srikanth Pilla. "Carbon Encapsulated Silicon for High-Capacity Durable Anodes." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 499. http://dx.doi.org/10.1149/ma2022-024499mtgabs.
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One of the biggest challenges of the near future is how to meet the increasing energy demand without any adverse environmental impact. Lithium-Ion batteries (LIBs) are one of the promising alternative energy storage systems to replace conventional non-rechargeable batteries. LIBs are becoming one of the most widely used energy storage devices because of their relatively high specific energy density (~300 Wh/kg), excellent stability over a wide temperature range, and lower cost than other battery systems. Intense research is in progress to increase the capacity of anode electrodes for realizing high-energy LIBs. In this context, silicon (Si) has a great potential to replace commercial graphitic anode active materials mainly due to its high theoretical specific capacity (4200 mAh/g) and low working potential (0.37 to 0.45 V vs. Li/Li+). To harness and maintain a high capacity from Si-based anodes, we must deal with two main challenges: (i) volume changes of Si (>300%) during charging and discharging, which cause pulverization of the material and loss of electrical contact, and (ii) unstable growth of solid-electrolyte interphase (SEI) layer, which can cause early degradation of performance in Si-anode batteries. To overcome these challenges, different approaches have been taken. This includes developing graphite/Si anodes with limited amounts of Si (<30 wt.%), conformal coating of Si active materials (e.g., CVD carbon coating), etc. However, these challenges still could not be fully overcome. To advance the use of Si materials in LIB anodes, we developed a viable technology to create a hybrid silicon-carbon material, called Si@C, in which a soybean-derived carbon cloud protects Si nanoparticles during the battery operation. We employed soybean oil in a scalable oil-in-water emulsion polymerization technique to produce Si-containing polymeric particles. In this method, we emulsified two immiscible solutions. One contains a homogeneous Si mixture in epoxidized soybean oil (ESO), and another contains a uniform dispersion of ball-milled lignin or soyhull powders in water. Citric acid, a crosslinking agent, was used to help polymerize the ESO and integrate carbon-rich lignin/soyhull with polymerized particles. The final Si@C product was achieved by carbonizing the polymerized solid product at 500 °C (under argon) and ball milling to get a fine powder. Several Si@C hybrid materials containing 20 wt.% to 50 wt.% Si were successfully prepared and utilized for anode preparation. Electrodes were made by coating a slurry of Si@C active material, carbon black, and binder with a mass ratio of 60:20:20 onto an ion-permeable Bucky Paper (BP, a flexible and conductive paper made of carbon nanotubes). Anodes with different binding systems were prepared to determine an appropriate binder for Si@C based batteries. The 2032-type coin cells were assembled for battery testing using 1M LiPF6 in EC:DMC in a volume ratio of 1:1 as the electrolyte, Li chips as the counter electrode, and Celgard 2325 as the separator. The coin cells were cycled at a current rate of 0.1C (420 mA/gSi) over the potential range of 0.01 – 1.0 V at room temperature. Battery results showed that Si@C hybrid materials increased the capacity of Si anodes by a factor of >2. At Si mass loading of 1.0 mg/cm2, implementing our carbon cloud approach led to an increase in the discharge capacity of anodes from 0.5 mAh (corresponding to anode with bare Si) to >1.0 mAh (corresponding to anode with Si@C hybrids). Results from battery cycling at 0.1C demonstrated excellent capacity retention of >95% after 130 cycles for anodes prepared using our Si@C active materials. The Si content of Si@C hybrid particles was also found to be an influential factor in the cycling performance of anodes. Finally, we observed that the use of water-based polyacrylic acid (PAA) and carboxymethyl cellulose (CMC) binders improve the electrochemical performance of Si@C based anodes. These water-based binders are ideal for preparing Si-based slurries, and the need for using toxic solvents (e.g., NMP) to prepare slurries can be averted. In conclusion, we innovated a viable technology that uses biomass (soybean oil and soyhulls) to enhance Si-based batteries' performance. We demonstrated that our Si@C materials with a carbon cloud protecting the Si nanoparticles are promising active materials to improve the capacity and cycling stability of LIB anodes.
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Shen, Huilin, Qilin Wang, Zheng Chen, Changru Rong, and Danming Chao. "Application and Development of Silicon Anode Binders for Lithium-Ion Batteries." Materials 16, no. 12 (June 8, 2023): 4266. http://dx.doi.org/10.3390/ma16124266.
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The use of silicon (Si) as a lithium-ion battery’s (LIBs) anode active material has been a popular subject of research, due to its high theoretical specific capacity (4200 mAh g−1). However, the volume of Si undergoes a huge expansion (300%) during the charging and discharging process of the battery, resulting in the destruction of the anode’s structure and the rapid decay of the battery’s energy density, which limits the practical application of Si as the anode active material. Lithium-ion batteries’ capacity, lifespan, and safety can be increased through the efficient mitigation of Si volume expansion and the maintenance of the stability of the electrode’s structure with the employment of polymer binders. The main degradation mechanism of Si-based anodes and the methods that have been reported to effectively solve the Si volume expansion problem firstly are introduced. Then, the review demonstrates the representative research work on the design and development of new Si-based anode binders to improve the cycling stability of Si-based anode structure from the perspective of binders, and finally concludes by summarizing and outlining the progress of this research direction.
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Cora, Saida, and Niya Sa. "Mechanisms of Si Stabilization for Future Anode Design." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 359. http://dx.doi.org/10.1149/ma2022-024359mtgabs.
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Silicon owing to its abundance, low working potential and high theoretical specific capacity has been regarded as one of the promising anode materials for the next generation lithium-ion batteries (LIBs). The bottleneck of Si anode practical application is its large volume variation and formation of reactive silicide species at the anode/electrolyte interface during lithiation which result in continuous SEI formation and consumption of active electrolyte components. The new electrolyte design strategies have shown to stabilize the Si electrode via an in situ electrochemical formation of a metastable ternary Li-Mg-Si phase. In this study, the effect of electrolyte modification on the dynamic formation of solid electrolyte interphase (SEI) on Si anode is investigate in the pre-lithiation versus post-lithiation stages of electrochemical cycling. In addition, combined EQCM-EIS are used to investigate the charge transfer mechanism and the resistivity of the surface film at various stages of cycling. The understanding of the stabilization effect of Mg salt on Si surface chemistry may have a great impact on the development of Si-based anodes for lithium-ion batteries.
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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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Liu, Guoshun, Xuhui Liu, Xingdong Ma, Xiaoqi Tang, Xiaobin Zhang, Jianxia Dong, Yunfei Ma, Xiaobei Zang, Ning Cao, and Qingguo Shao. "High-Performance Dual-Ion Battery Based on Silicon–Graphene Composite Anode and Expanded Graphite Cathode." Molecules 28, no. 11 (May 23, 2023): 4280. http://dx.doi.org/10.3390/molecules28114280.
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Dual-ion batteries (DIBs) are a new kind of energy storage device that store energy involving the intercalation of both anions and cations on the cathode and anode simultaneously. They feature high output voltage, low cost, and good safety. Graphite was usually used as the cathode electrode because it could accommodate the intercalation of anions (i.e., PF6−, BF4−, ClO4−) at high cut-off voltages (up to 5.2 V vs. Li+/Li). The alloying-type anode of Si can react with cations and boost an extreme theoretic storage capacity of 4200 mAh g−1. Therefore, it is an efficient method to improve the energy density of DIBs by combining graphite cathodes with high-capacity silicon anodes. However, the huge volume expansion and poor electrical conductivity of Si hinders its practical application. Up to now, there have been only a few reports about exploring Si as an anode in DIBs. Herein, we prepared a strongly coupled silicon and graphene composite (Si@G) anode through in-situ electrostatic self-assembly and a post-annealing reduction process and investigated it as an anode in full DIBs together with home-made expanded graphite (EG) as a fast kinetic cathode. Half-cell tests showed that the as-prepared Si@G anode could retain a maximum specific capacity of 1182.4 mAh g−1 after 100 cycles, whereas the bare Si anode only maintained 435.8 mAh g−1. Moreover, the full Si@G//EG DIBs achieved a high energy density of 367.84 Wh kg−1 at a power density of 855.43 W kg−1. The impressed electrochemical performances could be ascribed to the controlled volume expansion and improved conductivity as well as matched kinetics between the anode and cathode. Thus, this work offers a promising exploration for high energy DIBs.
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Abe, Yusuke, Ippei Saito, Masahiro Tomioka, Mahmudul Kabir, and Seiji Kumagai. "Effects of Excessive Prelithiation on Full-Cell Performance of Li-Ion Batteries with a Hard-Carbon/Nanosized-Si Composite Anode." Batteries 8, no. 11 (November 2, 2022): 210. http://dx.doi.org/10.3390/batteries8110210.
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The effects of excessive prelithiation on the full-cell performance of Li-ion batteries (LIBs) with a hard-carbon/nanosized-Si (HC/N-Si) composite anode were investigated; HC and N-Si simply mixed at mass ratios of 9:1 and 8:2 were analyzed. CR2032-type half- and full-cells were assembled to evaluate the electrochemical LIB anode behavior. The galvanostatic measurements of half-cell configurations revealed that the composite anode with an 8:2 HC/N-Si mass ratio exhibited a high capacity (531 mAh g−1) at 0.1 C and superior current-rate dependence (rate performance) at 0.1–10 C. To evaluate the practical LIB anode performance, the optimally performing composite anode was used in the full cell. Prior to full-cell assembly, the composite anodes were prelithiated via electrochemical Li doping at different cutoff anodic specific capacities (200–600 mAh g−1). The composite anode was paired with a LiNi0.5Co0.2Mn0.3O2 cathode to construct full-cells, the performance of which was evaluated by conducting sequential rate and cycling performance tests. Prelithiation affected only the cycling performance, without affecting the rate performance. Excellent capacity retention was observed in the full-cells with prelithiation conducted at cutoff anodic specific capacities greater than or equal to 500 mAh g−1.
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Yi, Ran, Sujong Chae, Yaobin Xu, Hyung-Seok Lim, Dusan Velickovic, Xiaolin Li, Qiuyan Li, Chongmin Wang, and Ji-Guang Zhang. "Scalable Synthesis of High Performance Silicon Anode by Impregnation of Pitch in Nanoporous Silicon." ECS Meeting Abstracts MA2022-02, no. 6 (October 9, 2022): 629. http://dx.doi.org/10.1149/ma2022-026629mtgabs.
Full textAbstract:
Silicon (Si) has been regarded as one of the most promising anode materials for the next generation LIBs with high energy density because it has 10 times higher theoretical specific capacity (4200 mAh/g) than that of graphite. However, severe volume change (~300%) of Si during lithiation and delithiation hinders the practical application of Si anode by 1) particle fracture and pulverization, 2) disintegration of electrode, and 3) continuous electrolyte-decomposition at the newly exposed Si surface. A novel process has been developed for the preparation of porous Si/C composite-based anode which demonstrate highly stable cycling stability. The enabling factor is a wet chemical, low temperature pitch coating process that uses readily available, low-cost, and abundant precursors. The porous Si nanostructure can be preserved by impregnating petroleum pitch before high-temperature treatment. A full cell with 80 wt% pitch-derived carbon/nanoporous Si in the anode has been demonstrated with 80% capacity retention after 450 cycles. Low swelling in both particle and electrode levels has also been observed. It is expected that the unique process developed in this work is also applicable for the development of other alloying-type anodes that require preservation of the desired nanostructures during high temperature treatment.
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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.
Full textAbstract:
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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Merazga, Saloua, Fatima Boudeffar, Bouaoua Achouak, Amina Larabi, Mourad Mebarki, Malika Berouaken, and Noureddine Gabouze. "Electrochemical Performances Ti4Ti5O12/Si Composite Anodes for Li-Ion Batteries." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 213. http://dx.doi.org/10.1149/ma2023-022213mtgabs.
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LTO /Si anode material for lithium-ion batteries were successfully synthesized by two-step hydrothermal method and ball milling synthesis , using tetrabutyl titanate, lithium acetate,silicone powder. In this work, LTO/Si composites with different weight ratios (50%,70%) were prepared and tested as anodes of Li-Ion Batteries.The electrochemical properties of the electrodes were investigated using by cyclic voltammetry , charge-discharge galvanostatic and impedance spectroscopy .Both the anodic and cathodic peaks from LTO and silicon were seen in the composites.LTO/SI Composites with higher Si contents (LTO =30 %et Si = 70%) have higher specific capacity .the results confirme that This material can be used as a high-power anode material in lithium-ion batteries.
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Zhang, Xian, Jingzheng Weng, Chengxi Ye, Mengru Liu, Chenyu Wang, Shuru Wu, Qingsong Tong, Mengqi Zhu, and Feng Gao. "Strategies for Controlling or Releasing the Influence Due to the Volume Expansion of Silicon inside Si−C Composite Anode for High-Performance Lithium-Ion Batteries." Materials 15, no. 12 (June 16, 2022): 4264. http://dx.doi.org/10.3390/ma15124264.
Full textAbstract:
Currently, silicon is considered among the foremost promising anode materials, due to its high capacity, abundant reserves, environmental friendliness, and low working potential. However, the huge volume changes in silicon anode materials can pulverize the material particles and result in the shedding of active materials and the continual rupturing of the solid electrolyte interface film, leading to a short cycle life and rapid capacity decay. Therefore, the practical application of silicon anode materials is hindered. However, carbon recombination may remedy this defect. In silicon/carbon composite anode materials, silicon provides ultra-high capacity, and carbon is used as a buffer, to relieve the volume expansion of silicon; thus, increasing the use of silicon-based anode materials. To ensure the future utilization of silicon as an anode material in lithium-ion batteries, this review considers the dampening effect on the volume expansion of silicon particles by the formation of carbon layers, cavities, and chemical bonds. Silicon-carbon composites are classified herein as coated core-shell structure, hollow core-shell structure, porous structure, and embedded structure. The above structures can adequately accommodate the Si volume expansion, buffer the mechanical stress, and ameliorate the interface/surface stability, with the potential for performance enhancement. Finally, a perspective on future studies on Si−C anodes is suggested. In the future, the rational design of high-capacity Si−C anodes for better lithium-ion batteries will narrow the gap between theoretical research and practical applications.
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Shan, Yunpeng, Junzhang Wang, Zhou Xu, Shengchi Bai, Yingting Zhu, Xiaoqi Wang, and Xingzhong Guo. "Bi-Continuous Si/C Anode Materials Derived from Silica Aerogels for Lithium-Ion Batteries." Batteries 9, no. 11 (November 10, 2023): 551. http://dx.doi.org/10.3390/batteries9110551.
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Poor cycling performance caused by massive volume expansion of silicon (Si) has always hindered the widespread application of silicon-based anode materials. Herein, bi-continuous silicon/carbon (Si/C) anode materials are prepared via magnesiothermic reduction of silica aerogels followed by pitch impregnation and carbonization. To fabricate the expected bi-continuous structure, mesoporous silica aerogel is selected as the raw material for magnesiothermic reduction. It is successfully reduced to mesoporous Si under the protection of NaCl. The as-obtained mesoporous Si is then injected with molten pitch via vacuuming, and the pitch is subsequently converted into carbon at a high temperature. The innovative point of this strategy is the construction of a bi-continuous structure, which features both Si and carbon with a cross-linked structure, which provides an area to accommodate the colossal volume change of Si. The pitch-derived carbon facilitates fast lithium ion transfer, thereby increasing the conductivity of the Si/C anode. It can also diminish direct contact between Si and the electrolyte, minimizing side reactions between them. The obtained bi-continuous Si/C anodes exhibit excellent electrochemical performance with a high initial discharge capacity of 1481.7 mAh g−1 at a current density of 300 mA g−1 and retaining as 813.5 mAh g−1 after 200 cycles and an improved initial Coulombic efficiency of 82%. The as-prepared bi-continuous Si/C anode may have great potential applications in high-performance lithium-ion batteries.
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Park, Hui Gyeong, Mincheol Jung, Shinyoung Lee, Woo-Jin Song, and Jung-Soo Lee. "Radical-Scavenging Activatable and Robust Polymeric Binder Based on Poly(acrylic acid) Cross-Linked with Tannic Acid for Silicon Anode of Lithium Storage System." Nanomaterials 12, no. 19 (September 30, 2022): 3437. http://dx.doi.org/10.3390/nano12193437.
Full textAbstract:
The design of a novel binder is required for high-capacity silicon anodes, which typically undergo significant changes during charge/discharge cycling. Hence, in this study, a stable network structure was formed by combining tannic acid (TAc), which can be cross-linked, and poly(acrylic acid)(PAA) as an effective binder for a silicon (Si) anode. TAc is a phenolic compound and representative substance with antioxidant properties. Owing to the antioxidant ability of the C-PAA/TAc binder, side reactions during the cycling were suppressed during the formation of an appropriate solid–electrolyte interface layer. The results showed that the expansion of a silicon anode was suppressed compared with that of a conventional PAA binder. This study demonstrates that cross-linking and antioxidant capability facilitate binding and provides insights into the behavior of binders for silicon anodes. The Si anode with the C-PAA/TAc binder exhibited significantly improved cycle stability and higher Coulombic efficiency in comparison to the Si anode with well-established PAA binders. The C-PAA/TAc binder demonstrated a capacity of 1833 mA h g−1Si for 100 cycles, which is higher than that of electrodes fabricated using the conventional PAA binder. Therefore, the C-PAA/TAc binder offers better electrochemical performance.
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Wang, Ying, Wei Ruan, Ren Heng Tang, Fang Ming Xiao, Tai Sun, and Ling Huang. "Preparation and Electrochemical Properties of Si@C/Graphite Composite as Anode for Lithium-Ion Batteries." Key Engineering Materials 807 (June 2019): 74–81. http://dx.doi.org/10.4028/www.scientific.net/kem.807.74.
Full textAbstract:
In this study, Si@C/Graphite composite anodes were synthesized through spray drying and pyrolysis using silica, artificial graphite, and two kinds of organics (phenolic resin or pitch). The Si@PR-C/Graphite exhibits enhanced electrochemical performance for lithium-ion batteries. The first charge-discharge specific capacity is 512.8mAh/g and 621.8mAh/g, respectively, the initial coulombic efficiency is 82.5% at 100mA/g, and its capacity retention rate reached as high as 85.4% with the capacity fade rate of less than 0.18% per cycle after 85 cycles. The Si@PI-C/Graphite also presents excellent discharge specific capacity of 702.8mAh/g with the capacity retention rate of 76.9% after 30 cycles. Mechanisms for high electrochemical performances of the Si@C/Graphite composite anode are discussed. It found that the enhanced electrochemical performance due to the formation of core/shell microstructure. These encouraging experimental results suggest that proper organic carbon source has great potential for improvement of electrochemical properties of pure silicon as anode. Key words:lithium-ion batteries; anode; Si@C/Graphite composite; electrochemical performance
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Chen, Yanxu, Yajing Yan, Xiaoli Liu, Yan Zhao, Xiaoyu Wu, Jun Zhou, and Zhifeng Wang. "Porous Si/Fe2O3 Dual Network Anode for Lithium–Ion Battery Application." Nanomaterials 10, no. 12 (November 25, 2020): 2331. http://dx.doi.org/10.3390/nano10122331.
Full textAbstract:
Benefiting from ultra-high theoretical capacity, silicon (Si) is popular for use in energy storage fields as a Li–ion battery anode material because of its high-performance. However, a serious volume variation happens towards Si anodes in the lithiation/delithiation process, triggering the pulverization of Si and a fast decay in its capacity, which greatly limits its commercial application. In our study, a porous Si/Fe2O3 dual network anode was fabricated using the melt-spinning, ball-milling and dealloying method. The anode material shows good electrochemical performance, delivering a reversible capacity of 697.2 mAh g−1 at 200 mA g−1 after 100 cycles. The high Li storage property is ascribed to the rich mesoporous distribution of the dual network structure, which may adapt the volume variation of the material during the lithiation/delithiation process, shorten the Li–ion diffusion distance and improve the electron transport speed. This study offers a new idea for developing natural ferrosilicon ores into the porous Si-based materials and may prompt the development of natural ores in energy storage fields.
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Khomenko, Volodymyr, Viacheslav Barsukov, and Ilona Senyk. "Electrochemical Properties of Advanced Anodes for Lithium-Ion Batteries Based on Carboxymethylcellulose as Binder." Key Engineering Materials 559 (June 2013): 49–55. http://dx.doi.org/10.4028/www.scientific.net/kem.559.49.
Full textAbstract:
Electrochemical properties and possibilities of manufacturing the anodes based on water-soluble binders such as carboxymethylcellulose (CMC) have been investigated in order to create prerequisites for development of “green” technologies for recyclability of LIBs components. In this work an advanced anode was designed. A kind of nanosized carbon coated Si composite was synthesized. The charge/discharge test reveals that the advanced anode shows a reversible capacity of 600 mAh/g. The improved performance was ascribed to the carbon shell of Si and CMC binder. The binder CMC buffers the expansion of the Si and the improved electric contact between the active material and copper current collector.
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Khomenko, Volodymyr, Kostiantyn Lykhnytskyi, Viacheslav Barsukov, and Vitalii Chaban. "Composite Catalysts towards Oxygen Reduction in Aqueous Solutions." Key Engineering Materials 559 (June 2013): 57–62. http://dx.doi.org/10.4028/www.scientific.net/kem.559.57.
Full textAbstract:
Electrochemical properties and possibilities of manufacturing the anodes based on water-soluble binders such as carboxymethylcellulose (CMC) have been investigated in order to create prerequisites for development of “green” technologies for recyclability of LIBs components.In this work an advanced anode was designed. A kind of nanosized carbon coated Si composite was synthesized. The charge/discharge test reveals that the advanced anode shows a reversible capacity of 600 mAh/g. The improved performance was ascribed to the carbon shell of Si and CMC binder. The binder CMC buffers the expansion of the Si and the improved electric contact between the active material and copper current collector.
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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.
Full textAbstract:
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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Patel, Yashkumar, Anjaliben Vanpariya, and Indrajit Mukhopadhyay. "Electrochemical Synthesis of Nano-Structured Si and Graphene Composite for Li Ion Battery." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 257. http://dx.doi.org/10.1149/ma2023-022257mtgabs.
Full textAbstract:
The application of lithium-ion batteries is widespread across a variety of sectors, such as portable electronic gadgets, mobile phones, new electric car batteries, and many others. Silicon–Graphene (SiG) anodes are among the sophisticated anode materials that have been used in lithium-ion batteries. These anodes have been widely researched because of their high capacity, strong operating potential, environmental friendliness and great abundance. SiG anodes have shown a lot of promise as a potential anode material for lithium-ion batteries [1]. This is due to the fact that they have solved many issues that were present in Si anodes, including particle pulverization, shedding and failures of electrochemical performance during lithiation and delithiation. Nevertheless, there are still certain issues that need to be improved, such as low initial discharge efficiency, poor conductivity and poor cycle performance. This research focuses on presenting a unique approach that may be used to address the issues associated with Si anode materials. An electrodeposition method that only needs a single unit operation, is applied in the process of constructing composites of SiG from G-1M SiCl4 in [BMIm]Tf2N ionic liquid (IL) [2]. In SiG composites, both silicon and graphene have been seen to have a layered structure (Fig.1 a). The SiG anode displays a specific charge/discharge capacity of 1133/ 2272 mAhg-1 at the first cycle and it drops to 676/ 737 mAhg-1 at the conclusion of 100 cycle at 0.2C (Fig.1b), which demonstrates a robust cycle ability at a moderate rate. The present work will thus discuss on the development of SiG composite by electrochemical method for its utility as negative electrode material in Li ion battery. References: Huang, Z. et al. Binder-free graphene/carbon nanotube/silicon hybrid grid as freestanding anode for high capacity lithium ion batteries. Compos. A 84, 386–392 (2016). Anjali Vanpariya, Kashinath Lellala, Dharini Bhagat, Indrajit Mukhopadhyay*, Electrochemical deposition of Si nano-spheres from water contaminated ionic liquid at room temperature: Structural evolution and growth mechanism, J. Electroanal. Chem., 910 (2022) 116175-116181. Figure 1
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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.
Full textAbstract:
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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Yang, Zhenzhen, Stephen E. Trask, Xianyang Wu, and Brian J. Ingram. "Effect of Si Content on Extreme Fast Charging Behavior in Silicon–Graphite Composite Anodes." Batteries 9, no. 2 (February 16, 2023): 138. http://dx.doi.org/10.3390/batteries9020138.
Full textAbstract:
Commercial Li-ion batteries typically incorporate a small amount of high-capacity silicon (Si)-based materials in the composite graphite-based anode to increase the energy density of the battery. However, very little is known about the effects of Si on the fast-charging behavior of composite anodes. Herein, we examine the effects of the Si/graphite ratio in the composite anode on the fast-charging behavior of full cells. We show that addition of Si increases the rate capability from 1C to 8C and improves the capacity retention in early cycles at 6C due to reduced overpotential in constant current charging cycles. The impacts of Si content on fast-charging aging were identified by Post-Test characterization. Despite realizing benefits of available capacity and reduced Li plating at 6C, silicon–electrolyte interactions lead the time-dependent cell performance to fade quickly in the long term. The Post-Test analysis also revealed the thickening of the electrode and nonuniform distribution of electrolyte decomposition products on the Si-containing anodes, as well as the organic-rich solid electrolyte interphase (SEI), which are the factors behind cell degradation. Our study sheds insight on the advantages and disadvantages of Si/graphite composite anodes when they are used in fast-charging applications and guides further research in the area by designing an optimized composition of Si incorporated in a mature graphite matrix.
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Li, Kefan, Xiang Li, Liang Yuan, Zewen Han, Mengkui Li, Rui Ji, Yixin Zhan, and Kai Tang. "High-Performance Porous pSi/Ag@C Anode for Lithium-Ion Batteries." Processes 12, no. 5 (May 17, 2024): 1021. http://dx.doi.org/10.3390/pr12051021.
Full textAbstract:
Silicon represents one of the most attractive anode materials in lithium-ion batteries (LIBs) due to its highest theoretical specific capacity. Thus, there is a most urgent need to prepare Si-based nano materials in a very efficient way and develop some reasonable approaches for their modification in order to resolve the short-falls of Si anodes, which include both low conductivity and huge volume changes during intercalation of lithium ions. In this work, the kerf loss silicon (KL Si) from the photovoltaic industry has been used as an inexpensive Si source for the preparation of a porous silicon/silver/carbon composite (pSi/Ag@C) as an anode material. Porous silicon was embedded with Ag particles via the Ag-catalyzed chemical etching process, providing additional space to accommodate the large volume expansion of silicon. After carbon coating from polymerization of tannic acid on the surface of pSi/Ag, a high-speed conductive network over the surface of silicon was built and contributed to enhancing the electrochemical performance of the anode. The pSi/Ag@C electrode discharge capacity maintained at a stable value of 665.3 mAh g−1 after 100 cycles under 0.5 A g−1 and exhibited good rate performance. Therefore, this study recommends that the method is very promising for producing a silicon anode material for LIBs from KL Si.
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Lee, Jungho, and Suguru Noda. "One-minute deposition of micrometre-thick porous Si anodes for lithium ion batteries." RSC Advances 5, no. 4 (2015): 2938–46. http://dx.doi.org/10.1039/c4ra11681j.
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3–14 μm-thick porous Si anodes were vapor-deposited on Cu current collectors in 10–60 s and discharge capacities of 1000 mA h gSi−1 and 0.66 mA h cmanode−2 were achieved for the 50th cycle.
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Leonova, Natalia M., Anastasia M. Leonova, Oleg A. Bashirov, Alexey S. Lebedev, Alexey A. Trofimov, and Andrey V. Suzdaltsev. "C/SiC-based anodes for lithium-ion current sources." Electrochemical Energetics 23, no. 1 (March 21, 2023): 41–50. http://dx.doi.org/10.18500/1608-4039-2023-23-1-41-50.
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Compositions of ultrafine Si and C particles are promising anode materials for lithium-ion power sources with improved energy characteristics. In the work, samples of lithium-ion power sources with an anode made of ultrafine SiC fibers, as well as mixtures of SiC fibers with graphite (C/SiC) and electrolytically deposited submicron silicon fibers (C/Si/SiC) were fabricated and studied for energy characteristics. The working ability of the mixtures obtained during lithiation/delithiation was shown, and the main energy characteristics of the investigated anode half-cells were determined. After 100 cycles, the SiC anode reached a discharge capacity of 180 and 138 mA·h/g at a charge current of C/20 and C, respectively. Anodes made of mixtures (wt%) 29.5C-70.5SiC and 50Si-14.5C-35.5SiC show discharge capacities of 328 and 400 mA·h/g at a charge current of C/2. The Coulomb efficiency of all samples was above 99%.
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Yue, Chenghao, Yao Liu, Shaoliang Guan, Alireza Fereydooni, Yuexi Zeng, Zhijie Wei, Yonggang Wang, and Yimin Chao. "Optimising Hollow-Structured Silicon Nanoparticles for Lithium-Ion Batteries." Materials 16, no. 17 (August 28, 2023): 5884. http://dx.doi.org/10.3390/ma16175884.
Full textAbstract:
Silicon has been proven to be one of the most promising anode materials for the next generation of lithium-ion batteries for application in batteries, the Si anode should have high capacity and must be industrially scalable. In this study, we designed and synthesised a hollow structure to meet these requirements. All the processes were carried out without special equipment. The Si nanoparticles that are commercially available were used as the core sealed inside a TiO2 shell, with rationally designed void space between the particles and shell. The Si@TiO2 were characterised using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). The optimised hollow-structured silicon nanoparticles, when used as the anode in a lithium-ion battery, exhibited a high reversible specific capacity over 630 mAhg−1, much higher than the 370 mAhg−1 from the commercial graphite anodes. This excellent electrochemical property of the nanoparticles could be attributed to their optimised phase and unique hollow nanostructure.
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Lin, Yueqiang, Bin Qi, Zhiyuan Li, Su Zhang, Tong Wei, and Zhuangjun Fan. "Low-cost micron-sized silicon/carbon anode prepared by a facile ball-milling method for Li-ion batteries." Advances in Engineering Technology Research 9, no. 1 (January 10, 2024): 330. http://dx.doi.org/10.56028/aetr.9.1.330.2024.
Full textAbstract:
Commercially, Si nanoparticles (nano Si) are blended with graphite to construct high-capacity Si/C anodes. However, this strategy falls short because of the high cost of nano Si, serious pollution due to the use of organic solvent, and weak physical-electrical connection between graphite and Si. Herein, using low-cost micron-sized Si (μSi) and graphite as the raw materials, we proposed a facial ball-milling method to construct high-performance Si/C anode (μSi/C@CH) in which milled Si particles are protected both by graphite matrix and homogeneous chitosan-derived carbon layer. It is shown that the N and O atoms not only tend to coordinate with Li+, generating uniformly-distributed Li+ transport channels, but also improve the electrical conductivity of the anode materials. As a result, μSi/C@CH shows high cycling stability (376.7 mAh g-1 at 0.5 A g-1 after 500 cycles) and good rate capability of 120.2 mAh g-1 at 5 A g-1. This dual protection strategy facilitates the practical application of Si/C materials in high-energy density Li ion batteries (LIBs).
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Wang, Evelyna, Marco-Tulio F. Rodrigues, and Baris Key. "Operando NMR Characterization of Cycled and Calendar Aged Si Anodes." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 380. http://dx.doi.org/10.1149/ma2023-022380mtgabs.
Full textAbstract:
Replacing graphite anodes with Si anodes can greatly increase the capacity of current Li-ion batteries. Detailed characterization of Si lithiation reactions, solid electrolyte interphase (SEI) formation, and reversibility are therefore active areas of research. Solid-state nuclear magnetic resonance (NMR) spectroscopy is useful for characterizing different local environments within Si anodes as well as differentiating surface and bulk environments. Furthermore, non-invasive and non-destructive NMR methods can reveal metastable LixSi phases or SEI species forming on (dis)charge that may be too reactive to detect via ex situ methods. Here, we use an in situ and in operando NMR methodology to characterize full pouch cells comprising of Si anodes and NMC cathodes. We can observe changes in the relative amounts of Li in different environments within the same Si anode before/during/after charge & discharge and with various amounts of cycling or calendar aging using in situ 7Li NMR. The pouch cells used in our in situ NMR study are comparable to pouch cells made using mid- to large-scale fabrication methods as opposed to laboratory scale; in other words, challenges of cell-to-cell variability are minimized. We hypothesize “trapped” lithiated phases formed in the Si anode no longer contribute to electrochemical cycling and thus limit capacity in subsequent cycles/aging. We also characterized the SEI/surface species in situ with aging via 13C NMR measurements, identifying reactions of lithium silicides with electrolyte solvents and their subsequent decomposition.
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Kong, Xiangzhong, Ziyang Xi, Linqing Wang, Yuheng Zhou, Yong Liu, Lihua Wang, Shi Li, Xi Chen, and Zhongmin Wan. "Recent Progress in Silicon−Based Materials for Performance−Enhanced Lithium−Ion Batteries." Molecules 28, no. 5 (February 22, 2023): 2079. http://dx.doi.org/10.3390/molecules28052079.
Full textAbstract:
Silicon (Si) has been considered to be one of the most promising anode materials for high energy density lithium−ion batteries (LIBs) due to its high theoretical capacity, low discharge platform, abundant raw materials and environmental friendliness. However, the large volume changes, unstable solid electrolyte interphase (SEI) formation during cycling and intrinsic low conductivity of Si hinder its practical applications. Various modification strategies have been widely developed to enhance the lithium storage properties of Si−based anodes, including cycling stability and rate capabilities. In this review, recent modification methods to suppress structural collapse and electric conductivity are summarized in terms of structural design, oxide complexing and Si alloys, etc. Moreover, other performance enhancement factors, such as pre−lithiation, surface engineering and binders are briefly discussed. The mechanisms behind the performance enhancement of various Si−based composites characterized by in/ex situ techniques are also reviewed. Finally, we briefly highlight the existing challenges and future development prospects of Si−based anode materials.
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An, Yonghao, Brandon C. Wood, Jianchao Ye, Yet-Ming Chiang, Y. Morris Wang, Ming Tang, and Hanqing Jiang. "Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design." Physical Chemistry Chemical Physics 17, no. 27 (2015): 17718–28. http://dx.doi.org/10.1039/c5cp01385b.
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A novel strategy is developed to mitigate lithiation-induced fracture in crystalline Si anodes by deliberately designing anisometric anode morphologies to counteract the anisotropy in the crystalline/amorphous interface velocity.
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Cao, Xiao Zhou, Zhu Xian Qiu, Zhong Ning Shi, Xian Wei Hu, Yun Gang Ban, and Zhao Wen Wang. "Anti-Oxidation and Anti-Corrosion Properties of Al-Si Metal Anodes." Materials Science Forum 546-549 (May 2007): 1149–52. http://dx.doi.org/10.4028/www.scientific.net/msf.546-549.1149.
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Al-Si metal anode was fabricated by cold-press sintering with Al and Si as embedded powder in argon atmosphere. The anti-oxidation in the air and anti-corrosion in molten cryolite properties of Al-Si metal anode at high temperature were examined. The experimental results showed that the oxidation kinetics curve obeyed the parabolic law. The corrosion behavior Al-Si metal anode was studied in electrolysis test. The electrolyte consisted of Na3AlF6(90 wt%),CaF2(5 wt%) and Al2O3(5 wt%) which corresponded to molecular ratio of 2.4. The results indicated that the cell voltage was stable and the electric polarized corrosion rate was higher than the static corrosion rate of metal anode. SEM photographs showed an oxidation film formed in the surface of Al-Si metal anode which can obstruct the further corrosion in molten cryolite. It may be concluded that Al-Si metal anode has good combination property and can replace the carbon anode in the aluminum cell.
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Thi, May Tran, Chulsoo Kim, Seokhun Kwon, Hyunil Kang, Jang Myoun Ko, Junghyun Kim, and Wonseok Choi. "Investigation of the Properties of Anode Electrodes for Lithium–Ion Batteries Manufactured Using Cu, and Si-Coated Carbon Nanowall Materials." Energies 16, no. 4 (February 15, 2023): 1935. http://dx.doi.org/10.3390/en16041935.
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The fabrication of high-capacity, binder-free Li–ion battery anodes using a simple and efficient manufacturing process was reported in this research. The anode material for lithium–ion batteries utilized is a combination of two-dimensional (2D) carbon nanowalls (CNWs) and Cu nanoparticles (improved rate performance and capacity retention) or Si (high capacity) nanoparticles. A methane (CH4) and hydrogen (H2) gas mixture was employed to synthesize CNWs on copper foil through microwave plasma-enhanced chemical vapor deposition (PECVD). The Cu or Si nanoparticles were then deposited on the CNW surface using an RF magnetron sputtering equipment with four-inch targets. To analyze the electrochemical performance of the LIBs, CR2032 coin-type cells were fabricated using anode materials based on CNWs and other components. It was confirmed that the Cu−CNW demonstrates improved rate performance, increased specific capacity, and capacity retention compared with traditional anodes. Additionally, CNW combined with Si nanoparticles has enhanced the capacity of LIB and minimized volume changes during LIB operation.
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Meng, Shirley. "Si Anode for All Solid State Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 249. http://dx.doi.org/10.1149/ma2022-023249mtgabs.
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The development of silicon anodes for lithium-ion batteries has been largely impeded by poor interfacial stability against liquid electrolytes. I will show how to enable the operation of a 99.9 weight % microsilicon anode by using the interface passivating properties of sulfide solid electrolytes. Advanced interface and bulk characterization, and quantification of interfacial components, showed that such an approach eliminates continuous interfacial growth and irreversible lithium losses. Microsilicon full cells were assembled and found to achieve high areal current density, wide operating temperature range, and high areal loadings for the different cells. The promising performance can be attributed to both the desirable interfacial property between microsilicon and sulfide electrolytes and the distinctive chemomechanical behavior of the lithium-silicon alloy. I will also discuss a few exciting future directions for nanosilicon with solid state electrolytes.
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Zhou, Xiangyang, Chucheng Luo, Jing Ding, Juan Yang, and Jingjing Tang. "WSi2 nanodot reinforced Si particles as anodes for high performance lithium-ion batteries." CrystEngComm 22, no. 39 (2020): 6574–80. http://dx.doi.org/10.1039/d0ce01047b.
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Zuo, Yezhan, Xingyu Xiong, Zhenzhong Yang, Yihui Sang, Haolin Zhang, Fanbo Meng, and Renzong Hu. "Engineering Nano-Sized Silicon Anodes with Conductive Networks toward a High Average Coulombic Efficiency of 90.2% via Plasma-Assisted Milling." Nanomaterials 14, no. 8 (April 10, 2024): 660. http://dx.doi.org/10.3390/nano14080660.
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Si-based anode is considered one of the ideal anodes for high energy density lithium-ion batteries due to its high theoretical capacity of 4200 mAh g−1. To accelerate the commercial progress of Si material, the multi-issue of extreme volume expansion and low intrinsic electronic conductivity needs to be settled. Herein, a series of nano-sized Si particles with conductive networks are synthesized via the dielectric barrier discharge plasma (DBDP) assisted milling. The p-milling method can effectively refine the particle sizes of pristine Si without destroying its crystal structure, resulting in large Brunauer–Emmett–Teller (BET) values with more active sites for Li+ ions. Due to their unique structure and flexibility, CNTs can be uniformly distributed among the Si particles and the prepared Si electrodes exhibit better structural stability during the continuous lithiation/de-lithiation process. Moreover, the CNT network accelerates the transport of ions and electrons in the Si particles. As a result, the nano-sized Si anodes with CNTs conductive network can deliver an extremely high average initial Coulombic efficiency (ICE) reach of 90.2% with enhanced cyclic property and rate capability. The C-PMSi-50:1 anode presents 615 mAh g−1 after 100 cycles and 979 mAh g−1 under the current density of 5 A g−1. Moreover, the manufactured Si||LiNi0.8Co0.1Mn0.1O2 pouch cell maintains a high ICE of >85%. This work may supply a new insight for designing the nano-sized Si and further promoting its commercial applications.
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Terechshenko, A., A. Sanbayeva, M. R. Babaa, A. Nurpeissova, and Z. Bakenov. "Spray-Pyrolysis Preparation of Li4Ti5O12/Si Composites for Lithium-Ion Batteries." Eurasian Chemico-Technological Journal, no. 1 (February 20, 2019): 69. http://dx.doi.org/10.18321/ectj793.
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This paper introduces the novel anode material which is Li4Ti5O12/Si prepared by gas-stated method, mainly spray-pyrolysis technique. The literature review performed in this paper revealed two main components which can be potentially mixed into the efficient anode material. Silicon (Si) has the highest possible capacity of 4200 mAh g-1 among all commonly used anodes. Due to its ‘zero-strain’ (<1% volume change) properties and stable cycling, Li4Ti5O12 (LTO) is considered as a promising anode for lithium ion batteries. Combination of these two anode materials is considered as a promising approach to prepare a high performance composite anode. The precursor solution consisted of homogeneous mixture of lithium nitrate and titanium tetraisopropoxide dissolved in deionized water with equimolar concentration of 0.5 M. The aerosol formation was performed at nitrogen environment and the droplets were carried into the quartz tube reactor at the flowrate of 4 L min-1. The rector temperature was held at 800 °C. The spray-pyrolysis synthesis was performed as one-step operation, excluding the need of calcination of as-prepared powders, and continuous process by the mean of peristaltic pump. The as-prepared powders had wide size distribution from nanometers to microns. The materials obtained had well-crystallized structure with insignificant amount of impurities. The powders were analyzed by the following analytical equipment: 1) the presence of Li4Ti5O12 and Si in the obtained composite was confirmed by X-ray diffraction technique (XRD); 2) The structure and morphology of LTO and Si molecules were observed and studied with Scanning Electron Microscopy (SEM).
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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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Kloker, Gabriele, Dragoljub Vrankovic, Martin Frey, and Montaha Anjass. "Enabling Si-Dominant Anodes with Focus on Binder." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2499. http://dx.doi.org/10.1149/ma2022-0272499mtgabs.
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Since current chemistries in lithium ion batteries (LIBs) including graphite anode reached their energy density limits, a promising candidate on anode side is the abundantly available silicon with its enormous capacity, but showing several failure mechanisms based on its extensive swelling (>300%). This leads to excessive solid electrolyte interphase (SEI) formation and electrode delamination during cycling, which can be reduced by the modification of the active material itself, e.g. carbon-embedded silicon (Si/C), but still these materials show the same failure mechanisms in a less pronounced manner. Regarding the costs and availability, the next generation anode is desired to be based on metallurgical silicon, where one promising path to enable Si-dominant anodes is the design of advanced binder systems to maintain a stable network around the active material during cycling. However, in most studies new binders are mainly tested in electrodes with low active material content and low loadings while lacking of full cell data, which makes it impossible to estimate the capability and influence of the binder to mitigate the failure mechanisms in full cell operation. In this work, several modifications of the binder are combined with commercial Si/C material and bare micro-sized silicon with 100% silicon as active material. The electrodes are tested in half coin cells and small full pouch cells with ~60 mAh capacity. To examine the performance in detail and understand the underlying failure mechanisms, post-mortem analysis was conducted. The already commonly used polyacrylic acid (PAA) can be further adapted to the respective anode active material (AAM) via partial neutralization with e.g. LiOH to tune the interaction with the AAM and reduce the first cycle losses due to the reaction of the carboxylic groups with lithium. Nevertheless, the influence of PAA/LiPAA on the failure mechanisms and maintenance of the electrode, especially on full cell basis, are not yet fully understood. In this work, the effect of the partial neutralization on the full cell performance of a NMC811-Si/C cell is shown with the anode consisting of 91.5% Si/C material, 8% binder and 0.5% conductive additive (single-wall carbon nanotubes SWCNTs). The full cells show 3.5% higher FCE with 70% neutralized LiPAA in comparison to acidic PAA in the anode, while maintaining the same cycle life.
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Morris, Louis Vincent, Cesar Ortiz-Ledon, and Robert J. Hamers. "Adapting Simultaneous in Operando Electrochemical Quartz Crystal Microbalance (EQCM) and Electrochemical Impedance Spectroscopy (EIS) to Studies of SEI Layer Formation on Amorphous Silicon Anodes." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 171. http://dx.doi.org/10.1149/ma2022-012171mtgabs.
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Lithium-ion Batteries (LIBs) are the electrochemical energy storage technology of choice for an incredible range of technologies, from handheld consumer electronics to electric vehicles. Since their introduction, the application of these batteries has been limited by their energy density, which is in turn currently gated by the low theoretical energy density of the graphite anodes that are standard in the field. Si has long been targeted as a next generation anode material, with a theoretical energy density almost 10 times larger than graphite, however uncontrolled electrolyte decomposition on its surface has caused poor cycle life and low columbic efficiencies in Si-containing cells1. In this work, a new class of organosilicon (OS) additives were introduced to the Si anode literature and their effect on the first-cycle electrochemistry on model anode surface was explored using in operando electrochemical quartz crystal microbalancing (EQCM) and electrochemical impedance spectroscopy (EIS). Ex situ x-ray photoemission spectroscopy (XPS) was also used to investigate the differences in chemical composition of solid electrolyte interface (SEI) layers formed in the presence and absence of additive. EQCM-EIS experiments demonstrated an increase in cell impedance early in the cycle, which lead to the suppression of early electrolyte decomposition on the model anode surface. Subsequently, lithiation and delithiation proceeded more efficiently and with lower impedance in additive-treated cells. Finally, XPS investigations of the SEI composition revealed that OS-treated cells create thinner SEI layers that were richer in LiF and contained less organic material than cells without OS. (1) Jin, Y.; Zhu, B.; Lu, Z.; Liu, N.; Zhu, J. Challenges and Recent Progress in the Development of Si Anodes for Lithium-Ion Battery. Adv. Energy Mater. 2017, 1700715, 1–17. https://doi.org/10.1002/aenm.201700715.
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Zhang, Chuan-Zhu, Lin-Jie Xie, Yan Tang, You Li, Jun-Cheng Jiang, and An-Chi Huang. "Thermal Safety Evaluation of Silane Polymer Compounds as Electrolyte Additives for Silicon-Based Anode Lithium-Ion Batteries." Processes 10, no. 8 (August 11, 2022): 1581. http://dx.doi.org/10.3390/pr10081581.
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The capacity fading and thermal safety issues caused by the volume effect of Si-based anodes and unstable solid electrolyte interphase (SEI) films during long-term cycling limit its large-scale application. In this study, silane polymer compound (2-cyanoethyl) triethoxysilane (TCN) was selected as an electrolyte additive to improve the reversibility and thermal safety of Si-based anode lithium-ion batteries (LIBs). TCN prevented the thermal interaction between the vitiated anode and electrolyte, and the onset temperature of the thermal reaction increased from 122.22 to 127.07 °C, as demonstrated by the results of thermogravimetric analysis and differential scanning calorimetry. The thermal stability of lithiated anodes containing various electrolytes was then assessed using a range of thermo-kinetic models. The results revealed that the activation energy of Si-based lithiated anodes increased from 68.46 to 91.32 kJ/mol, while the thermal hazard greatly decreased. Additionally, the electrochemical test and characterization results showed that TCN helped generate a stable SEI coating with more Li2CO3 components, which improved the cells’ cycle stability. This study provides a new reference for the growth of LIBs with high security and energy density.