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Ali, Yasir, Noman Iqbal, Imran Shah, and Seungjun Lee. "Mechanical Stability of the Heterogenous Bilayer Solid Electrolyte Interphase in the Electrodes of Lithium–Ion Batteries." Mathematics 11, no. 3 (January 19, 2023): 543. http://dx.doi.org/10.3390/math11030543.
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Mechanical stability of the solid electrolyte interphase (SEI) is crucial to mitigate the capacity fade of lithium–ion batteries because the rupture of the SEI layer results in further consumption of lithium ions in newly generated SEI layers. The SEI is known as a heterogeneous bilayer and consists of an inner inorganic layer connecting the particle and an outer organic layer facing the electrolyte. The growth of the bilayer SEI over cycles alters the stress generation and failure possibility of both the organic and inorganic layers. To investigate the probability of mechanical failure of the bilayer SEI, we developed the electrochemical-mechanical coupled model with the core–double-shell particle/SEI layer model. The growth of the bilayer SEI is considered over cycles. Our results show that during charging, the stress of the particle changes from tensile to compressive as the thickness of bilayer SEI increases. On the other hand, in the SEI layers, large compressive radial and tensile tangential stress are generated. During discharging, the compressive radial stress of the bilayer SEI transforms into tensile radial stress. The tensile tangential and radial stresses are responsible for the fracture and debonding of the bilayer SEI, respectively. As the thickness ratio of the inorganic to organic layers increases, the fracture probability of the inorganic layer increases, while that of the organic layer decreases. However, the debonding probability of both layers is decreased. In addition, the SEI covering large particles is more vulnerable to fracture, while that covering small particles is more susceptible to debonding. Therefore, tailoring the thickness ratio of the inorganic to organic layers and particle size is important to reduce the fracture and debonding of the heterogeneous bilayer SEI.
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Lucht, Brett L. "(Invited) Optimization of Carbonate Electrolytes for Lithium Metal Anodes." ECS Meeting Abstracts MA2023-02, no. 5 (December 22, 2023): 830. http://dx.doi.org/10.1149/ma2023-025830mtgabs.
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A solid electrolyte interphase (SEI) is generated on the anode of lithium ion batteries during the first few charging cycles. While the SEI generated for LiPF6/carbonate based electrolytes is stable on graphite anodes, the stability of the SEI is poor for LiPF6/carbonate based electrolytes with lithium metal anodes. However, modification of the carbonate based electrolytes via incorporation of alternative salts and/or electrolyte additives significantly improves the stability of the SEI and the cycle life of lithium metal anodes. Investigations of the SEI structure have been conducted via a combination of XPS, IR-ATR, SEM, and TEM. Mechanisms for the generation of the complicated mixture of products are presented along with the differences in the SEI structure and function.
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Yao, Koffi, Rownak Jahan Mou, Sattajit Barua, and Daniel P. Abraham. "(Digital Presentation) Unraveling of the Morphology and Chemistry Dynamics in the FEC-Generated Silicon Anode SEI across Delithiated and Lithiated States." ECS Meeting Abstracts MA2023-02, no. 8 (December 22, 2023): 3289. http://dx.doi.org/10.1149/ma2023-0283289mtgabs.
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The silicon solid electrolyte interphase (SEI) faces cyclical cracking and reconstruction due to the ~350% volume expansion of Si which leads to shortened cell life during electrochemical cycling. Understanding the SEI morphology/chemistry and more importantly its dynamic evolution from delithiated and lithiated states is paramount to engineering a stable Si anode. Fluoroethylene carbonate (FEC) is a preferred additive with widely demonstrated enhancement of the Si cycling. Thus, insights into the effects of FEC on the dynamics of the resulting SEI may provide hints toward engineering the Si interface. Herein, ATR-FTIR, AFM, tip IR, and XPS probing all show pronounced relative invariance of the FEC-generated SEI compared to the FEC-free SEI between adjacent lithiated and delithiated states beyond the formation cycles. The SEI of Si thin film model surfaces in the baseline 1 M LiPF6 in EC:EMC (1:1) undergoes major morphological and chemical speciation swings between half-cycles while comparatively the SEI upon addition of FEC displays far less dynamic evolution. This morphology and chemistry stability of the FEC-SEI supports the enhanced cycling stability of silicon anodes in FEC-containing electrolytes. The experimental evidence gathered suggests that the FEC-SEI invariance is enabled by an elastomeric polycarbonate matrix that preserves the SEI integrity against the expansion of silicon upon lithiation. In turn, less electrolyte-consuming reconstruction occurs which manifests as and high LiF content from one half-cycle to the next. This work provides critical insights to enhance the silicon anode stability via targeted SEI engineering, namely that LiF protected by an elastomeric protective matrix may be key to buffering the unavoidable mechanical disruption. Figure 1
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Mesmin, C., and J. ‐O Liljenzin. "Determination of H2TPTZ22+Stability Constant by TPTZ Solubility in Nitric Acid." Solvent Extraction and Ion Exchange 21, no. 6 (January 11, 2003): 783–95. http://dx.doi.org/10.1081/sei-120025922.
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Ji, Yuchen, Luyi Yang, and Feng Pan. "In-Situ Probing the Origin of Interfacial Instability of Na Metal Anode." ECS Meeting Abstracts MA2023-02, no. 5 (December 22, 2023): 832. http://dx.doi.org/10.1149/ma2023-025832mtgabs.
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The chemical-mechanical stability of solid–electrolyte interphase (SEI) is probably the most critical factor determining the performance of alkali metal anode (Li, Na, etc.) in secondary batteries. Although extensive advanced characterization methods have been carried out to study SEI layers of Na metal anode, including solid state nuclear magnetic resonance1, 2, cryogenic transmission electron microscopy3, etc., the structural/componential evolution of SEI is still an uncharted territory due to its transient formation process and complicated components. In this work, we systematically analyze the SEI formation and dissolution processes via jointly combining multiple in-situ characterization technologies. By revealing spatial-temporal resolved information of SEI evolution, the buried origin of chemical-mechanical instability of SEI in Na anode is further clarified, which provides valuable guidelines for SEI engineering. A dynamic SEI formation/dissolution model of Na metal anode is demonstrated as follow: Quantitative evaluation methods for the chemical instability (i.e., solubility) and mechanical instability (i.e., modulus) are designed. According to the mass variation in EQCM and the modulus measurement in in-situ AFM, we firstly quantitatively observe the chemical and mechanical stability evolution during SEI formation process. The dynamic evolution picture of SEI formation has been explicitly established. We discover the instantaneous electrochemical formation process of SEI is obviously divided into two stages based on the potential. It is revealed that the formation of efficient passivation layer anchored on Na surface during the 1st (passivating) stage (2.3 – 1 V vs Na/Na+) (Scheme 1 a-b) is the critical factor to construct stable SEI. In absence of passivation layer, the Na mental surface will trigger unrestricted electrolyte decomposition and homogenous components distribution during the subsequent (growing) stage. The dissolution model of SEI was revealed related to its spatial distribution of organics and inorganics. SEI with layered structure evolved from a compact passivation layer is found to have higher stability than that with homogenously distributed components. The inorganic species in the latter structure tend to detach from the SEI with the dissolution of organics, resulting in poor SEI chemical stability (Scheme 1 c and e). By contrast, SEIs with hierarchical structure growing based on the top of a passivation layer exhibits lower dissolution tendency (Scheme 1 d and f). The dynamic analysis of SEI evolution of Na anode presented in this work not only sheds light on how to construct a stable SEI, but also provides guiding significance in unveiling the seemingly complicated interfacial chemistry in batteries via a concerted characterization approach. References Gao, L.N., Chen, J.E., Chen, Q.L. et al. The chemical evolution of solid electrolyte interface in sodium metal batteries. Science Advances 8, 4606 (2022). Xiang, Y., Zheng, G., Liang, Z. et al. Visualizing the growth process of sodium microstructures in sodium batteries by in-situ 23Na MRI and NMR spectroscopy. Nat. Nanotechnol. 15, 883–890 (2020). Han, B., Zou, Y., Zhang, Z. et al. Probing the Na metal solid electrolyte interphase via cryo-transmission electron microscopy. Nat Commun 12, 3066 (2021). Figure 1
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Swallow, Jack E. N., Michael Fraser, Nis-Julian Kneusels, Jodie F. Charlton, Christopher G. Sole, Conor Phelan, Erik Björklund, et al. "Operando X-Ray Absorption Spectroscopy of Solid Electrolyte Interphase Formation on Silicon Anodes." ECS Meeting Abstracts MA2023-02, no. 5 (December 22, 2023): 825. http://dx.doi.org/10.1149/ma2023-025825mtgabs.
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Lithium-ion batteries (LIBs) are key to the transition from fossil fuels towards increased use of renewable energy sources. However, more widespread deployment requires improvements in energy density, cost and cycle-lifetime. Various cathode and anode materials are under consideration for next-generation LIBs, and the interfacial stability of these materials in contact with the electrolyte is a critical consideration. Interface-sensitive operando characterization techniques are thus urgently needed to reveal the reactions occurring in working batteries.1,2 The solid electrolyte interphase (SEI) that forms on Li-ion battery anodes is critical to their long-term performance, however observing SEI formation processes at the buried electrode-electrolyte interface is a significant challenge. Here we show that operando soft X-ray absorption spectroscopy in total electron yield mode can resolve the chemical evolution of the SEI during electrochemical formation in a Li-ion cell, with nm-scale interface sensitivity. O, F, and Si K-edge spectra, acquired as a function of potential, reveal when key reactions occur on high-capacity amorphous Si anodes cycled with and without fluoroethylene carbonate (FEC).3 Cross-referencing to cycling data, complementary bulk sensitive fluoresecent yield (FY) XAS measurements, and density functional theory (DFT) calculated spectra enables identification of the electrolyte and SEI species, and the dominant mechanisms of SEI formation. Without FEC present, LiF formation is detected at 0.6 V vs. Li/Li+ prior to significant lithiation of the a-Si, whilst at lower potentials the SEI grows in thickness with an increased contribution from organic components containing -C(=O)O- species. The observed sequential formation of inorganic and organic components is implicated in layering of the SEI. With FEC as an additive we see the onset of SEI formation at much higher potentials (1.0 V vs. Li/Li+), and attribute the improved cycle life seen with this additive to the rapid healing of SEI defects formed during delithiation. Operando TEY-XAS offers new insights into the formation mechanisms of electrode-electrolyte interphases and their stability for a wide variety of electrode materials and electrolyte formulations. References Wu et al. Phys. Chem. Chem. Phys. 2015, 17, 30229. Weatherup et al. Top. Catal. 2018, 61, 2085. Swallow et al. Nature Commun. 2022, 13, 6070.
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Westhead, Olivia, Matthew Spry, Zonghao Shen, Alexander Bagger, Hossein Yadegari, Silvia Favero, Romain Tort, et al. "Solvation and Stability in Lithium-Mediated Nitrogen Reduction." ECS Meeting Abstracts MA2022-02, no. 49 (October 9, 2022): 1929. http://dx.doi.org/10.1149/ma2022-02491929mtgabs.
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The lithium-mediated method of electrochemical nitrogen reduction, pioneered by Tsuneto et al1 then verified by Andersen et al2, is currently the sole paradigm capable of unequivocal electrochemical ammonia synthesis. Such a system could allow the production of green, distributed ammonia for use as fertiliser or a carbon-free fuel. However, despite great improvements in Faradaic efficiency and stability since just 20193, fundamental understanding of the mechanisms governing nitrogen reduction and other parasitic reactions is lacking. Lithium Ion Battery (LIB) research can provide insight; since both lithium-mediated electrochemical ammonia synthesis and LIBs utilise an organic solvent and lithium salt, both form a Solid Electrolyte Interphase (SEI), which is electronically insulating but ionically conducting, at the electrode surface. In LIBs, this is necessary to stabilize and cycle low potential materials4. In lithium-mediated ammonia synthesis, the SEI could also have a critical role in controlling the access of protons and other key reactants to the catalytically active sites and promoting greater selectivity toward nitrogen reduction to ammonia5. While some characterisation of the SEI has been carried out for the lithium-mediated nitrogen reduction system6, the literature still lacks holistic studies which aim to carefully characterise the bulk electrolyte and SEI components and link them to system performance. In this work we use insight from battery science to tackle a significant stability problem in lithium-mediated nitrogen reduction. The traditional electrolyte employed by Tsuneto et al. was 0.2 M LiClO4 in a 99:1 tetrahydrofuran to ethanol mix. While this system can produce ammonia, the working electrode potential becomes more negative over time. Our initial investigations show that this problem stems from an unstable SEI which becomes increasingly organic. Simply by raising the concentration of LiClO4 in the electrolyte, we vastly improve stability, as shown in figure 1(a), and boost Faradaic efficiency. Bulk electrolyte salt solvation properties are investigated through Raman spectroscopy, as shown in figure 1(b). Here we observe the emergence of a shoulder at around 930 cm-1 with increasing LiClO4 concentration, which we assign to the emergence of Contact-Ion-Pairs (CIPs) through comparison to Density Functional Theory calculations. These CIPs mean that perchlorate anion degradation products are more abundant in the formed SEI, as shown in our X-Ray Photoelectron Spectroscopy and Time-of-Flight Secondary Ion Mass spectrometry results. This more inorganic SEI protects the electrolyte against further degradation, preventing the working electrode drift to more negative potentials. We then link this behaviour to a peak observed in the Faradaic efficiency of ammonia synthesis at 0.6 M LiClO4 by also considering decreasing N2 solubility and diffusivity, as well as a more ionically conductive SEI, in an increasingly concentrated electrolyte. We also present never-before seen cross-sectional images of the SEI using cryogenic Focussed Ion Beam milling and Scanning Electron Microscopy, further aiding understanding of how salt solvation affects the morphology of the formed SEI and system performance. Our results emphasise the need to consider SEI properties in electrolyte design for lithium-mediated nitrogen reduction, as well as the need to balance desirable SEI properties with desirable bulk electrolyte properties. Tsuneto, A., Kudo, A. & Sakata, T. Efficient Electrochemical Reduction of N 2 to NH 3 Catalyzed by Lithium . Chemistry Letters vol. 22 851–854 (1993). Andersen, S. Z. et al. A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements. Nature 570, 504–508 (2019). Westhead, O., Jervis, R. & Stephens, I. E. L. Is lithium the key for nitrogen electroreduction? Science. 372, 1149–1150 (2021). Peled, E. & Menkin, S. Review—SEI: Past, Present and Future. J. Electrochem. Soc. 164, A1703–A1719 (2017). Singh, A. R. et al. Electrochemical Ammonia Synthesis—The Selectivity Challenge. ACS Catal. 7, 706–709 (2017). Li, K. et al. Enhancement of lithium-mediated ammonia synthesis by addition of oxygen. Science. 1597, 1593–1597 (2021). Figure 1
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Alexandratos, Spiro D., and Stephanie D. Smith. "High Stability Solvent Impregnated Resins: Metal Ion Complexation as a Function of Time." Solvent Extraction and Ion Exchange 22, no. 4 (December 31, 2004): 713–20. http://dx.doi.org/10.1081/sei-120038701.
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Wang, Menghao. "In Situ Formation of Dense Polymers as Artificial Protective Layers for Lithium Metal Anodes." Journal of Physics: Conference Series 2578, no. 1 (August 1, 2023): 012034. http://dx.doi.org/10.1088/1742-6596/2578/1/012034.
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Abstract In order to improve the stability and safety of lithium (Li) metal anodes, an innovative artificial solid electrolyte interface (SEI) film of Li Poly (tert-butyl acrylate-co-ethyl acrylate-co-methacrylic acid) (LiPTBEM) has been designed. This thin and uniformly artificial SEI is stable, which can suppress the continuous side reactions between the electrolyte and Li metal, improve the stability of modified Li metal anodes, and achieve better electrochemical performance. Symmetric batteries with LiPTBEM exhibit significantly improved cycling stability, indicating that LiPTBEM is a promising artificial SEI film.
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Guo, Xuyun, Xiaoqiong DU, Valeria Nicolosi, Biao Zhang, and Ye Zhu. "Tailoring Breathing Behaviour of Solid Electrolyte Interphases (SEIs) Unraveled by Cryo-TEM." ECS Meeting Abstracts MA2023-02, no. 5 (December 22, 2023): 882. http://dx.doi.org/10.1149/ma2023-025882mtgabs.
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The cycling stability of batteries is closely related to the dynamic evolution of solid electrolyte interphases (SEIs) in response to the discharging/charging processes. Here we utilize the state-of-the-art cryogenic transmission electron microscopy (cryo-TEM) and spectroscopy to probe the SEI breathing behaviour induced by discharging/charging on the conversion-type anode made of Fe2O3 quasi-cubes. The incorporation of the identical-location strategy allows us to track the evolution of same SEIs at different charge states, which unequivocally unravels SEI breathing featured by swelling (contracting) upon lithiation (de-lithiation), and the associated compositional change. Bare Fe2O3 anode develops an unstable SEI layer due to the intermixing with the lithiation product Li2O, which exhibits a large thickness variation upon breathing as well as excessive growth, causing substantial capacity fading within 100 cycles. A transition from organic to inorganic-type SEI is also identified upon cycling, which gives rise to significantly increased SEI resistance. To tailor the SEI behaviour, we apply N-doped carbon coating on Fe2O3 (Fe2O3@CN), which can effectively separate the lithiation product from SEI. A thinner and chemically more stable SEI layer develops on Fe2O3@CN, resulting in remarkably enhanced cycling stability compared to bare Fe2O3. Our work demonstrates the importance of understanding and optimizing the dynamic behaviour of SEIs to achieve better battery performance.
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Morasch, Robert, Hubert A. Gasteiger, and Bharatkumar Suthar. "Li-Ion Battery Material Impedance Analysis II: Graphite and Solid Electrolyte Interphase Kinetics." Journal of The Electrochemical Society 171, no. 5 (May 1, 2024): 050548. http://dx.doi.org/10.1149/1945-7111/ad48c0.
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Li-ion battery graphite electrodes form a solid-electrolyte-interphase (SEI) which is vital in protecting the stability and efficiency of the cell. The SEI properties have been studied extensively in the context of formation and additives, however studying its kinetic features after formation have been neglected. In this study we show the dynamic resistive behavior of the SEI after formation. Via electrochemical impedance spectroscopy measurements on Cu-foil after SEI formation we show how the SEI shows a potential-dependent resistance which can be explained by a change in charge carriers (Li+) in the SEI. Additional measurements on graphite exhibit a similar behavior and allow us to separate the charge transfer kinetics from the SEI resistance, showing that the SEI resistance is the dominating resistance in the graphite kinetics. Measurements on pre-formed electrodes also show how the SEI resistance changes when in contact with electrolyte of different LiPF6 salt concentrations, with the resistance decreasing for increasing salt concentrations. Ultimately, we show that the SEI resistance affects Li-plating by acting as an offset to the plating reaction but does not affect the nucleation overpotential itself.
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Guihua, Li, and Jin Zhen. "Global stability of an SEI epidemic model." Chaos, Solitons & Fractals 21, no. 4 (August 2004): 925–31. http://dx.doi.org/10.1016/j.chaos.2003.12.031.
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Kim, Ji-Wan, Myung-Keun Oh, Yeona Kim, Eun-Ji Kwon, Samuel Seo, Wonkeun Kim, Kyounghan Ryu, and Dong-Won Kim. "Enhancing Cycle Life of Lithium Metal Batteries By Regulating Solid-Electrolyte Interphase Using Gel Polymer Electrolyte." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 698. http://dx.doi.org/10.1149/ma2023-024698mtgabs.
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Lithium metal with high theoretical capacity and low redox potential is one of the promising anode materials for high energy density batteries. However, the lithium metal has safety problems and poor cycling performance, due to the growth of Li dendrite and side reactions between Li and electrolytes. One of the most effective strategies to stabilize Li metal is forming robust solid-electrolyte interphase (SEI). Recently, anion-derived and inorganic-rich SEI is known to be stable and ionic conductive, leading to good cycling stability. One of the most popular strategies to form durable SEI is to use the localized high-concentration electrolytes (LHCE) which construct an anion-derived SEI layer on Li metal. In this work, we synthesized LHCE-based gel polymer electrolytes to form a stable SEI layer and enhance cycling stability. Small amount of cross-linking agent was added into dimethoxyethane (DME)-based LHCE when synthesizing gel polymer electrolyte. The functional groups in cross-linking agents increase Li+ and anion interaction in the gel polymer electrolytes, resulting in formation of the stable SEI layer. The solvation structure and chemical composition of the SEI layer were investigated by density functional theory (DFT) calculation and spectroscopic analyses such as FT-IR, Raman, and XPS. The Li/NCM811 cells with LHCE-based gel polymer electrolyte were assembled for the cycling test, and they exhibited superior cycling performance than liquid electrolyte-based cells.
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Lim, Kyungmi, Marion Hagel, Kathrin Küster, Bernhard Fenk, Jürgen Weis, Ulrich Starke, Jelena Popovic, and Joachim Maier. "Chemical stability and functionality of Al2O3 artificial solid electrolyte interphases on alkali metals under open circuit voltage conditions." Applied Physics Letters 122, no. 9 (February 27, 2023): 093902. http://dx.doi.org/10.1063/5.0123535.
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We studied chemical stability of atomic layer deposition-grown Al2O3 artificial solid electrolyte interphases (SEIs) on lithium and sodium upon contact with liquid electrolyte by electrochemical impedance spectroscopy (EIS) and in the case of Li also by x-ray photoelectron spectroscopy. Both methods show that the formed Al2O3 is porous for all nominal thicknesses, and that the natural SEI grows in its pores and cracks. EIS shows that the porosity of the SEI on Na is higher than the one observed on Li, in particular at higher nominal thicknesses of Al2O3. The observed values of activation energies related to the transport through the SEI indicate either a denser natural SEI in the pores of Al2O3 and/or considerable space charge effect between Al2O3 and the SEI phase.
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Modolo, Giuseppe, and Stefan Seekamp. "HYDROLYSIS AND RADIATION STABILITY OF THE ALINA SOLVENT FOR ACTINIDE(III)/LANTHANIDE(III) SEPARATION DURING THE PARTITIONING OF MINOR ACTINIDES." Solvent Extraction and Ion Exchange 20, no. 2 (April 24, 2002): 195–210. http://dx.doi.org/10.1081/sei-120003021.
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Song, Xiaosheng, Shiyu Li, Xifei Li, Yaohui Zhang, Xiaobing Wang, Zhimin Bai, Hirbod Maleki Kheimeh Sari, Yong Zhao, and Jiujun Zhang. "A lattice-matched interface between in situ/artificial SEIs inhibiting SEI decomposition for enhanced lithium storage." Journal of Materials Chemistry A 8, no. 22 (2020): 11165–76. http://dx.doi.org/10.1039/d0ta00448k.
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Lattice-matched interfaces are introduced between the in situ SEI and the artificial LiAlO2 layer and demonstrated their substantial advantages in inhibiting the decomposition of the in situ SEI and boosting the cycling stability of LIBs.
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Xue, Yakui, Xinpeng Yuan, and Maoxing Liu. "Global stability of a multi-group SEI model." Applied Mathematics and Computation 226 (January 2014): 51–60. http://dx.doi.org/10.1016/j.amc.2013.09.050.
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Lahiri, Abhishek, Natalia Borisenko, Andriy Borodin, Mark Olschewski, and Frank Endres. "Characterisation of the solid electrolyte interface during lithiation/delithiation of germanium in an ionic liquid." Physical Chemistry Chemical Physics 18, no. 7 (2016): 5630–37. http://dx.doi.org/10.1039/c5cp06184a.
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The characterisation of the SEI layer revealed that LiTFSI–[Py1,4] is a relatively good ionic liquid based electrolyte for lithium batteries. However modifications in the electrolyte or a different anion might be necessary to improve the stability and composition of the SEI layer.
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Fan, Lishuang, Zhikun Guo, Yu Zhang, Xian Wu, Chenyang Zhao, Xun Sun, Guiye Yang, Yujie Feng, and Naiqing Zhang. "Stable artificial solid electrolyte interphase films for lithium metal anode via metal–organic frameworks cemented by polyvinyl alcohol." Journal of Materials Chemistry A 8, no. 1 (2020): 251–58. http://dx.doi.org/10.1039/c9ta10405d.
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Polyvinyl alcohol (PVA) as a “glue” to cement the metal organic framework (Zn-MOF) sheet as a reasonable artificial SEI film. The artificial SEI film can efficiently adapt to the changes of the volume during the cycle, significantly improve the stability of the Li metal anode.
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Beheshti, S. Hamidreza, Mehran Javanbakht, Hamid Omidvar, Hamidreza Behi, Xinhua Zhu, Mesfin Haile Mamme, Annick Hubin, Joeri Van Mierlo, and Maitane Berecibar. "Effects of Structural Substituents on the Electrochemical Decomposition of Carbonyl Derivatives and Formation of the Solid–Electrolyte Interphase in Lithium-Ion Batteries." Energies 14, no. 21 (November 4, 2021): 7352. http://dx.doi.org/10.3390/en14217352.
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The solid–electrolyte interphase (SEI), the passivation layer formed on anode particles during the initial cycles, affects the performance of lithium-ion batteries (LIBs) in terms of capacity, power output, and cycle life. SEI features are dependent on the electrolyte content, as this complex layer originates from electrolyte decomposition products. Despite a variety of studies devoted to understanding SEI formation, the complexity of this process has caused uncertainty in its chemistry. In order to clarify the role of the substituted functional groups of the SEI-forming compounds in their efficiency and the features of the resulting interphase, the performance of six different carbonyl-based molecules has been investigated by computational modeling and electrochemical experiments with a comparative approach. The performance of the electrolytes and stability of the generated SEI are evaluated in both half-cell and full-cell configurations. Added to the room-temperature studies, the cyclability of the NMC/graphite cells is assessed at elevated temperatures as an intensified aging condition. The results show that structural adjustments within the SEI-forming molecule can ameliorate the cyclability of the electrolyte, leading to a higher capacity retention of the LIB cell, where cinnamoyl chloride is introduced as a novel and more sustainable SEI forming agent with the potential of improving the LIB capacity retention.
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Schlaier, Jonas, Roman Fedorov, Shixian Huang, Yair Ein-Eli, Michael Schneider, Christian Heubner, and Alexander Michaelis. "Electrochemical Characterization of Artificial Solid Electrolyte Interphase Developed on Graphite Via ALD." ECS Meeting Abstracts MA2023-02, no. 60 (December 22, 2023): 2909. http://dx.doi.org/10.1149/ma2023-02602909mtgabs.
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During formation of Li-ion batteries, a ‘natural’ solid electrolyte interphase (SEI) is formed at the anode side by decomposition products of the electrolyte. The properties of the SEI are extremely decisive for the overall battery properties, such as rate capability and cycling stability. However, the SEI formation consumes Li, leading to so called ‘formation losses’ that can make up to 15% of the theoretical energy density of the battery. Several approaches have been presented to overcome formation losses while preserving excellent overall battery properties. Particularly, electrochemical prelithiation and the application of artificial SEIs prior cell assembly are considered to effectively reduced formation losses while improving the interfacial charge transfer properties and increasing cycling stability. Herein, the authors present an innovative approach of applying a multifunctional artificial SEI on anode material powders via consecutive atomic layer deposition (ALD) cycles. As a model system, graphite powder has been chosen to be modified and characterized. The resulting electrodes show substantially improved electrochemical performance in half cells and full cells, regarding initial capacity loss, CE and cycling stability. Furthermore, model electrodes consisting of a single layer of graphite particles were manufactured, which exclude the effects of a typical composite electrode and therefore reveal the intrinsic properties of the active material. Using this approach, the interfacial kinetics and the rate capability are investigated comparatively between pristine and ALD coated electrodes, revealing the impact of the artificial SEI on the materials level.
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Shen, B. H., S. Wang, and W. E. Tenhaeff. "Ultrathin conformal polycyclosiloxane films to improve silicon cycling stability." Science Advances 5, no. 7 (July 2019): eaaw4856. http://dx.doi.org/10.1126/sciadv.aaw4856.
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Electrochemical reduction of lithium ion battery electrolyte on Si anodes was mitigated by synthesizing nanoscale, conformal polymer films as artificial solid electrolyte interface (SEI) layers. Initiated chemical vapor deposition (iCVD) was used to deposit poly(1,3,5,7-tetravinyl-1,3,5,7-tetramethylcyclotetrasiloxane) (pV4D4) onto silicon thin film electrodes. pV4D4 films (25 nm) on Si electrodes improved initial coulombic efficiency by 12.9% and capacity retention over 100 cycles by 64.9% relative to untreated electrodes. pV4D4 coatings improved rate capabilities, enabling higher lithiation capacity at all current densities. Impedance spectroscopy showed that SEI resistance grew from 50 to 191 ohms in untreated Si and only 34 to 90 ohms in pV4D4-coated Si over 30 cycles. Post-cycling Fourier transform infrared and x-ray photoelectron spectroscopy showed that pV4D4 moderated electrolyte reduction and altered SEI composition, with LiF formation being favored. This work will guide further development of polymeric artificial SEIs to mitigate electrolyte reduction and enhance capacity retention in Si electrodes.
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Yu, Yikang, Hyeongjun Koh, Zhenzhen Yang, Eric A. Stach, and Jian Xie. "Revisiting Anode Fast-Charging Capability with Solid Electrolyte Interface Using Cryogenic Transmission Electron Microscopy." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 476. http://dx.doi.org/10.1149/ma2023-012476mtgabs.
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The Li+ ion diffusion through the solid electrolyte interphase (SEI) has been widely considered as one of the limiting steps for the Li fast (de)intercalation process. However, a comprehensive understanding of the kinetic limitation of SEI on anode fast-charging remains elusive. Using H-phase (monoclinic) Nb2O5 (H-Nb2O5) as the anode material, we comprehensively studied the fast charging behaviors on both “inorganic SEI free” and “inorganic-rich SEI” anodes with cryogenic transmission electron microscopy (cryo-TEM) and X-ray photoelectron spectroscopy (XPS). The results reveal that there is a negligible difference on the electrochemical performance including fast-charging capability and cycling stability between these H-Nb2O5 anodes in spite of significant discrepancy of SEI structure (e.g. thickness and chemical component). Further, it was observed using cryo-TEM that the discrete decoration of the individual inorganic particles (e.g. Li2O) and amorphous LiNxOy species in the direct SEI does not constitute a dense solid layer. From this study, we conclude a pore diffusion mechanism is dominated across the whole direct SEI layer with those porous organic components, which is extremely faster than the lithium ion knock-off diffusion in the inner inorganic components. Thus, the SEI structures have much less influence on the limitation of the lithium ion transport kinetics than those as commonly accepted if an inner dense inorganic layer is not formed. Our results provide a refreshed understanding on the fundamentals of the lithium ion transport in SEI, and will guide future design of battery materials for fast-charging.
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Lucht, Brett L. "(Invited) Electrolyte Oxidation and the Role of Crossover Species in Capacity Loss for Lithium Ion Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 195. http://dx.doi.org/10.1149/ma2022-012195mtgabs.
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Cycling lithiated metal oxides to high potential (>4.5 V vs Li) is of significant interest for the next generation of lithium ion batteries. Cathodes cycled to high potential suffer from rapid capacity fade due to a combination of thickening of the anode solid electrolyte interphase (SEI) and impedance growth on the cathode. While transition metal catalyzed degradation of the anode SEI has been widely proposed as a primary source of capacity loss, we propose a related acid induced degradation of the anode SEI. A systematic investigation of LiMn2O4, LiNi0.5Mn1.5O4, LiNi0.6Mn0.2Co0.2O2, and LiNi0.8Mn0.1Co0.1O2 cathodes will be presented. The role of potential on the generation of soluble acidic fluorophosphates crossover species and the impact of these species on the structure and stability of the SEI will be presented.
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Shi, Pengcheng, Xu Wang, Xiaolong Cheng, and Yu Jiang. "Progress on Designing Artificial Solid Electrolyte Interphases for Dendrite-Free Sodium Metal Anodes." Batteries 9, no. 7 (June 27, 2023): 345. http://dx.doi.org/10.3390/batteries9070345.
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Nature-abundant sodium metal is regarded as ideal anode material for advanced batteries due to its high specific capacity of 1166 mAh g−1 and low redox potential of −2.71 V. However, the uncontrollable dendritic Na formation and low coulombic efficiency remain major obstacles to its application. Notably, the unstable and inhomogeneous solid electrolyte interphase (SEI) is recognized to be the root cause. As the SEI layer plays a critical role in regulating uniform Na deposition and improving cycling stability, SEI modification, especially artificial SEI modification, has been extensively investigated recently. In this regard, we discuss the advances in artificial interface engineering from the aspects of inorganic, organic and hybrid inorganic/organic protective layers. We also highlight key prospects for further investigations.
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Cheng, Xin-Bing, and Qiang Zhang. "Dendrite-free lithium metal anodes: stable solid electrolyte interphases for high-efficiency batteries." Journal of Materials Chemistry A 3, no. 14 (2015): 7207–9. http://dx.doi.org/10.1039/c5ta00689a.
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A more superior cycling stability and a higher utilization ratio of the Li metal anode have been achieved by additive- and nanostructure-stabilized SEI layers. A profound understanding of the composition, internal structure, and evolution of the SEI film sheds new light on dendrite-free high-efficiency lithium metal batteries.
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Lenarcik, Beniamin, and Agnieszka Kierzkowska. "The Influence of Alkyl Chain Length on Stability Constants of Zn(II) Complexes with 1‐Alkylimidazoles in Aqueous Solutions and Their Partition Between Aqueous Phase and Organic Solvent." Solvent Extraction and Ion Exchange 22, no. 3 (December 31, 2004): 449–71. http://dx.doi.org/10.1081/sei-120030398.
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Clarke-Hannaford, Jonathan, Michael Breedon, Thomas Rüther, and Michelle J. S. Spencer. "Fluorinated Boron-Based Anions for Higher Voltage Li Metal Battery Electrolytes." Nanomaterials 11, no. 9 (September 14, 2021): 2391. http://dx.doi.org/10.3390/nano11092391.
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Lithium metal batteries (LMBs) require an electrolyte with high ionic conductivity as well as high thermal and electrochemical stability that can maintain a stable solid electrolyte interphase (SEI) layer on the lithium metal anode surface. The borate anions tetrakis(trifluoromethyl)borate ([B(CF3)4]−), pentafluoroethyltrifluoroborate ([(C2F5)BF3]−), and pentafluoroethyldifluorocyanoborate ([(C2F5)BF2(CN)]−) have shown excellent physicochemical properties and electrochemical stability windows; however, the suitability of these anions as high-voltage LMB electrolytes components that can stabilise the Li anode is yet to be determined. In this work, density functional theory calculations show high reductive stability limits and low anion–cation interaction strengths for Li[B(CF3)4], Li[(C2F5)BF3], and Li[(C2F5)BF2(CN)] that surpass popular sulfonamide salts. Specifically, Li[B(CF3)4] has a calculated oxidative stability limit of 7.12 V vs. Li+/Li0 which is significantly higher than the other borate and sulfonamide salts (≤6.41 V vs. Li+/Li0). Using ab initio molecular dynamics simulations, this study is the first to show that these borate anions can form an advantageous LiF-rich SEI layer on the Li anode at room (298 K) and elevated (358 K) temperatures. The interaction of the borate anions, particularly [B(CF3)4]−, with the Li+ and Li anode, suggests they are suitable inclusions in high-voltage LMB electrolytes that can stabilise the Li anode surface and provide enhanced ionic conductivity.
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Wu, Zhan-Yu, Li Deng, Jun-Tao Li, Sandrine Zanna, Antoine Seyeux, Ling Huang, Shi-Gang Sun, Philippe Marcus, and Jolanta Światowska. "Solid Electrolyte Interphase Layer Formation on the Si-Based Electrodes with and without Binder Studied by XPS and ToF-SIMS Analysis." Batteries 8, no. 12 (December 5, 2022): 271. http://dx.doi.org/10.3390/batteries8120271.
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The formation and evolution of the solid electrolyte interphase (SEI) layer as a function of electrolyte and electrolyte additives has been extensively studied on simple and model pure Si thin film or Si nanowire electrodes inversely to complex composite Si-based electrodes with binders and/or conductive carbon. It has been recently demonstrated that a binder-free Si@C-network electrode had superior electrochemical properties to the Si electrode with a xanthan gum binder (Si-XG-AB), which can be principally related to a reductive decomposition of electrolytes and formation of an SEI layer. Thus, here, the Si@C-network and Si-XG-AB electrodes have been used to elucidate the mechanism of SEI formation and evolution on Si-based electrodes with and without binder induced by lithiation and delithiation applying surface analytical techniques. The X-ray photoelectron spectroscopy and time-of-flight ion mass spectrometry results demonstrate that the SEI layer formed on the surface of the Si-XG-AB electrode during the discharge partially decomposes during the subsequent charging process, which results in a less stable SEI layer. Contrarily, on the surface of the Si@C-network electrode, the SEI shows less significant decomposition during the cycle, demonstrating its stability. For the Si@C-network electrode, initially, the inorganic and organic species are formed on the surface of the carbon shell and the silicon surface, respectively. These two parts of species in the SEI layer gradually grow and then fuse when the electrode is fully discharged. The behavior of the SEI layer on both electrodes corroborates with the electrochemical results.
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Zhao, Xvtong, Ying Chen, Hao Sun, Tao Yuan, Yinyan Gong, Xinjuan Liu, and Taiqiang Chen. "Impact of Surface Structure on SEI for Carbon Materials in Alkali Ion Batteries: A Review." Batteries 9, no. 4 (April 14, 2023): 226. http://dx.doi.org/10.3390/batteries9040226.
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Due to their low cost, suitable working potential and high stability, carbon materials have become an irreplaceable anode material for alkali ion batteries, such as lithium ion batteries, sodium ion batteries and potassium ion batteries. During the initial charge, electrolyte is reduced to form a solid electrolyte interphase (SEI) on the carbon anode surface, which is an electron insulator but a good ion conductor. Thus, a stable surface passivation is obtained, preventing the decomposition of electrolyte in the following cycles. It has been widely accepted that SEI is essential for the long-term performance of batteries, such as calendar life and cycle life. Additionally, the initial coulombic efficiency, rate capability as well as safety of the batteries are dramatically influenced by the SEI. Extensive research efforts have been made to develop advanced SEI on carbon materials via optimization of electrolytes, including solutes, solvents and additives, etc. However, SEI is produced via the catalytic decomposition of electrolyte by the surface of electrode materials. The surface structure of the carbon material is another important aspect that determines the structure and property of SEI, which little attention has been paid to in previous years. Hence, this review is dedicated to summarizing the impact of the surface structure of carbon materials on the composition, structure and electrochemical performance of the SEI in terms of surface atoms exposed, surface functionalization, specific surface area and pore structure. Some insights into the future development of SEI from the perspective of carbon surface are also offered.
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Wang, Donghai. "(Invited) Development of Interfacial Materials for High-Performance Battery Materials." ECS Meeting Abstracts MA2023-02, no. 1 (December 22, 2023): 71. http://dx.doi.org/10.1149/ma2023-02171mtgabs.
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Metal and alloy anode materials are the most promising anode for next-generation batteries. The interfacial instability in the electrochemical energy storage devices has been the primary issue hindering their practical application. In this talk, I will present approaches on de novo designing and architecting stable interphases on electrode materials using chemically and electrochemically active materials. The strategy works by introducing multiple functional components into the polymer composite which can bond to the Li-based material surface to participate in the formation of the SEI. The reinforced SEI shows much better stability than the SEI generated by the electrolyte additive strategy. The functional-material-derived interfaces/interphases present desirable ionic conductivity, density, homogeneity, and mechanical strength. The interfaces/interphases reinforced by the interfacial materials show much better stability than that reinforced by conventional strategies such as using electrolyte additive-commercially used solution to interface stability issues. Our findings open a new way to design stable electrochemically stable interfaces in electrode materials for next-generation electrochemical energy storage.
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Tranter, T. J., R. D. Tillotson, and T. A. Todd. "Laboratory‐Scale Column Testing Using Crystalline Silicotitanate (IONSIV™ IE‐911) for Removing Cesium from Acidic Tank Waste Simulant. 1: Cesium Exchange Capacity of a 15‐cm3Column and Dynamic Stability of the Exchange Media*." Solvent Extraction and Ion Exchange 23, no. 4 (July 2005): 583–93. http://dx.doi.org/10.1081/sei-200062611.
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Kung, Yu-Ruei, Cheng-Yao Li, Panitat Hasin, Chia-Hung Su, and Jeng-Yu Lin. "Effects of Butadiene Sulfone as an Electrolyte Additive on the Formation of Solid Electrolyte Interphase in Lithium-Ion Batteries Based on Li4Ti5O12 Anode Materials." Polymers 15, no. 8 (April 21, 2023): 1965. http://dx.doi.org/10.3390/polym15081965.
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In this study, butadiene sulfone (BS) was selected as an efficient electrolyte additive to stabilize the solid electrolyte interface (SEI) film on the lithium titanium oxide (LTO) electrodes in Li-ion batteries (LIBs). It was found that the use of BS as an additive could accelerate the growth of stable SEI film on the LTO surface, leading to the improved electrochemical stability of LTO electrodes. It can be supported by the BS additive to effectively reduce the thickness of SEI film, and it significantly enhances the electron migration in the SEI film. Consequently, the LIB-based LTO anode in the electrolyte containing 0.5 wt.% BS showed a superior electrochemical performance to that in the absence of BS. This work provides a new prospect for an efficient electrolyte additive for next-generation LIBs-based LTO anodes, especially when discharged to low voltage.
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Sarkar, Susmita, and Partha P. Mukherjee. "Electrolytes and Interfaces Driven Thermal Stability of Sodium-Ion Batteries." ECS Meeting Abstracts MA2022-02, no. 4 (October 9, 2022): 501. http://dx.doi.org/10.1149/ma2022-024501mtgabs.
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Recognizing the mandates in sustainability and material abundance, sodium-ion batteries hold great potential in being alternate chemistry for applications such as grid storage systems. Along with other performance matrices, the safety problem known as “thermal runaway” must be understood and overcome for the practical realization of sodium-ion batteries in countless applications. While the physiochemical properties of the model electrode materials play a major role in determining overall thermal stability, electrolyte-derived unstable solid electrolyte interphases (SEI) can also trigger early thermal instability. Since the sodium-ion battery has a highly soluble SEI layer, especially in carbonate electrolytes, it is essential to understand the thermal instability signatures of electrode-electrolyte interactions. So far, the interfacial driven thermal stability of sodium-ion battery electrodes remains largely unexplored. Herein, we aim to investigate the intrinsically stochastic and heterogeneous nature of the SEI layer, illustrating the role of carbonate and glyme solvents in determining the overall thermal stability of the cell. The fundamentals of the thermal failure issues explored in this work can pave the way toward building a safer sodium-ion battery.
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King, Laura J., Xu Hou, Erik J. Berg, and Maria Hahlin. "Investigating the Reaction Mechanism of Vinylene Carbonate Additive in Lithium Ion Batteries Using X-Ray Photoelectron Spectroscopy." ECS Meeting Abstracts MA2023-02, no. 65 (December 22, 2023): 3070. http://dx.doi.org/10.1149/ma2023-02653070mtgabs.
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The rechargeable Li-ion battery is an enabling technology which facilitates the electrification of the automotive industry and reduces the demand for fossil fuels. During the charge and discharge of a battery, a solid-electrolyte interphase (SEI) forms between the liquid electrolyte and the solid negative electrode as a result of electrolyte degradation. The chemical and physical stability and the functionality of the SEI is a key determining factor of battery performance. The chemical composition of the SEI is mainly controlled by the choice of solvent and salt used, but can be manipulated by the addition of electrolyte additives that influence the electrolyte degradation process. Vinylene carbonate (VC) is an additive used in many commercial Li-ion battery configurations. The addition of a small amount of VC to ethylene carbonate (EC) containing electrolytes has been demonstrated to drastically improve several performance metrics for batteries including cycle life, coulombic efficiencies, capacity retention and thermal stability. The success of VC is widely attributed to its ability to form a thinner, denser and more robust SEI, which better protects the electrode surface and prevents further electrolyte consumption. This improvement in stability has been linked to the presence of poly(VC) in the SEI, but the mechanism by which VC reacts in EC-containing electrolytes is still an area of ongoing study. Whilst computational methods have suggested several potential decomposition pathways of electrolytes containing VC, it is yet to be convincingly demonstrated experimentally. Whilst there is a general consensus about ‘What?’ forms in the SEI on the addition of VC to EC-containing solvent, this work aims to confirm ‘Where?’ these components are in the interface and the currently unanswered questions of ‘How?’ and ‘Why?’ they form. Using highly surface sensitive photoelectron spectroscopy (PES) measurements of the SEI deposited at various potentials, we identify the differences in composition and structure that result from the addition of VC additive to EC-containing electrolytes. The SEI formation is studied using a smooth Au surface as the model working electrode and a fluorine free EC:diethyl carbonate (DEC) (1:9) 1 M LiClO4 electrolyte in an attempt to isolate the impact of VC on the SEI. A potential step procedure allows analysis of the working electrode surface by PES at several progressively more negative potentials on the first charge. Through systematic variation of components such as the concentration of VC, the ratio of EC:DEC and swapping Au for other electrode materials such as Cu or Si, the interaction between VC, EC and the electrode surface is revealed. The differences in SEI composition and structure formed in each environment and at each potential step are correlated to quartz crystal microbalance (QCM) data in order to identify potential reaction mechanisms and formation processes. The results play a key role in understanding the reaction pathway of VC-containing electrolytes and will accelerate development of more efficient electrolyte additives.
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DeCaluwe, Steven C. "(Invited, Digital Presentation) Detailed Chemical Modeling of Solid Electrolyte Interphase Growth and Evolution." ECS Meeting Abstracts MA2022-01, no. 38 (July 7, 2022): 1660. http://dx.doi.org/10.1149/ma2022-01381660mtgabs.
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The solid electrolyte interphase (SEI) is a layer that forms at the anode-electrolyte interphase in lithium ion batteries. The layer forms due to voltage instability of the electrolyte at low anode potentials, but serves to passivate the electrolyte to protect against further uncontrolled decomposition. In theory, the SEI is self-limiting, but in reality, continued growth over the battery’s lifetime leads to capacity fade, poor rate capability, and eventually cell death. Though significant progress in recent years has improved the SEI’s function and stability, poor understanding of its most basic chemistry impedes “rational design” of SEI layers for advanced battery applications. Understanding and quantifying the elementary chemistry of the SEI is made challenging by the layer’s thickness (10s to ~100 nm), chemical sensitivity, mechanical fragility, and complex chemistry (upwards of 100 reactions have been proposed). For these reasons, These factors combine to make studying the fundamental chemistry of SEI growth and evolution a significant challenge. Both the computational tools to model the SEI’s complex chemistry and the experimental data required to validate such models are all too rare. This talk will provide an overview of recent efforts to model the fundamental electrochemistry of SEI growth and evolution. The simulations are based on a continuum-scale, finite-volume framework, and leverage the open-source software package Cantera to enable efficient simulation of arbitrarily complex electrochemical mechanisms. Simulation results, as in Figure 1, are validated against two operando measurements of the SEI grown on a non-intercalating tungsten anode: depth profiling via neutron reflectometry (NR), and SEI mass uptake data via quartz crystal microbalance with dissipation (QCM-D) taken during cyclic voltammetry cycling. Interrogation of the detailed model results provide insights into the complex phenomena controlling initial SEI growth, and validation against NR and QCM-D data identify prominent reaction pathways and key chemical species present in the SEI. Finally, we will conclude by discussing future steps, includuing transferring mechanistic insights to new scales, geometries, and chemistries, and coupling models with inputs from atomistic simulations. Figure 1
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Abioye, A. I., O. J. Peter, F. A. Oguntolu, A. F. Adebisi, and T. F. Aminu. "GLOBAL STABILITY OF SEIR-SEI MODEL OF MALARIA TRANSMISSION." Advances in Mathematics: Scientific Journal 9, no. 8 (August 15, 2020): 5305–17. http://dx.doi.org/10.37418/amsj.9.8.2.
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Fan, Xiulin, Xiao Ji, Fudong Han, Jie Yue, Ji Chen, Long Chen, Tao Deng, Jianjun Jiang, and Chunsheng Wang. "Fluorinated solid electrolyte interphase enables highly reversible solid-state Li metal battery." Science Advances 4, no. 12 (December 2018): eaau9245. http://dx.doi.org/10.1126/sciadv.aau9245.
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Solid-state electrolytes (SSEs) are receiving great interest because their high mechanical strength and transference number could potentially suppress Li dendrites and their high electrochemical stability allows the use of high-voltage cathodes, which enhances the energy density and safety of batteries. However, the much lower critical current density and easier Li dendrite propagation in SSEs than in nonaqueous liquid electrolytes hindered their possible applications. Herein, we successfully suppressed Li dendrite growth in SSEs by in situ forming an LiF-rich solid electrolyte interphase (SEI) between the SSEs and the Li metal. The LiF-rich SEI successfully suppresses the penetration of Li dendrites into SSEs, while the low electronic conductivity and the intrinsic electrochemical stability of LiF block side reactions between the SSEs and Li. The LiF-rich SEI enhances the room temperature critical current density of Li3PS4to a record-high value of >2 mA cm−2. Moreover, the Li plating/stripping Coulombic efficiency was escalated from 88% of pristine Li3PS4to more than 98% for LiF-coated Li3PS4. In situ formation of electronic insulating LiF-rich SEI provides an effective way to prevent Li dendrites in the SSEs, constituting a substantial leap toward the practical applications of next-generation high-energy solid-state Li metal batteries.
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Kumar, Mukesh, and Tharamani C. Nagaiah. "Tuning the Interfacial Chemistry for Stable and High Energy Density Aqueous Sodium-Ion/Sulfur Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 612. http://dx.doi.org/10.1149/ma2023-024612mtgabs.
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The environmental-related issues arising from the fossil fuel assorted industrial revolution and worldwide development have prompted the quest for rechargeable batteries. In these predicaments, lithium-ion batteries (LIBs) took ownership to reshape our lives. However, the limited abundance, non-uniform geographical distribution and severe flammability of organic electrolytes, increase the uncertainty over their large-scale application. Recently, aqueous rechargeable sodium-ion batteries (ARSIBs) have gained considerable curiosity for large-scale energy storage due to their much-assured safety, environment friendliness, high-rate capacity, and low cost. However, the prospects of ARSIBs seeing commercial success remained remote due to the narrow water stability window (1.23 V), which translates into low cell voltage (< 1.6 V), low energy density (< 70 Wh Kg-1), and compromised cycling stability. The aforesaid dilemmas can be resolved by generating a protective layer known as a solid electrolyte interface (SEI) like in organic electrolytes. However, the SEI concept in aqueous electrolytes is relatively unexplored, as water dissociation leads to O2 and H2, and will enhance the parasitic reactions. The SEI formed in WiSE due to salt reduction is often inhomogeneous with a porous mosaic structure and is susceptible to mechanical cracking, and increase the overall cost. Hence, high-capacity electrodes and high voltage electrolytes capable of forming a stable SEI are urgently required to fulfill the dream of the large-scale application of ARSIBs. Recently low cost, highly abundant sulfur-based electrode material has attracted significant research attention due to its high theoretical capacity (1675 mA h g-1) and energy density. However, sluggish sulfur redox kinetics, acute polysulfide shutting, dendritic growth on the metal-based anode and low conductivity of sulfur and its discharge products proves to be a major roadblock for its commercialization. Utilizing abundant sulfur in an aqueous electrolyte along with abundant Na+ can resolve the kinetics and conductivity anxieties and leads to a new greener and safer Na-ion/S batteries chemistry. However lower order polysulfide dissolution in water is more feasible, leading to the rapid capacity decay and active sulfur loss due to H2S formation. Polysulfide dissolution is an interfacial mechanism occurring at the electrode-electrolyte interface and depends on both electrode and electrolyte merits. Therefore, an effective approach will be to couple efficient sulfur host with an electrolyte capable of generating a stable SEI on the electrode surface to prevent the direct attack of water on polysulfide. Herein we have explored urchin-like CoWO4 as a sulfur host coupled with Na-W-U-D electrolyte. The CoWO4 exhibits high conductivity, strong chemical interaction for sulfur and its discharge products, and urchin-like morphology having exposed edges facilitate the charge transport results in excellent polysulfide redox kinetics. The high voltage Na-W-U-D electrolyte was prepared by mixing NaClO4, urea, and N, N-dimethylformamide DMF in 1:2:1 ratio in water. Each component in the electrolyte plays an important role. Urea has very high water solubility and tends to form stable SEI, while DMF has a high dielectric constant, good solvation ability, and develop stabilize SEI. As a result, Na-W-U-D shows a stability window close to the 3.1 V regime due to reduced water activity resulting from complex ion solvent interaction and stable and uniform SEI formation, consisting of Na2CO3, polyurea, and reduction products of DMF. Despite the addition of DMF, non-flammable features of aqueous electrolytes remain well maintained. Herein for the first time, the SEI concept was successfully used for the aq. Na-ion/S battery. We discovered that the lower water activity of Na-W-U-D electrolyte hindered polysulfide dissolution and stable SEI prevent the direct attack of water on polysulfide and results in extended cycling stability. At the same time, the urchin-like CoWO4 host enhances the sluggish polysulfide redox kinetics and provides an abundant anchoring site for polysulfide adsorption. We investigate the effect of time, C-rate, depth of discharge, and dissolved oxygen on polysulfide dissolution and self-discharge of the negative electrode. The high electrode capacity combined with the safety and stable SEI of Na-W-U-D electrolyte translated into a record high initial capacity of 834 mA h g-1 w.r.t sulfur, with remarkable cycling stability up to 500 cycles @ 0.5 C. Post analysis by SEM and XPS, evident that the stable SEI consists of Na2CO3, polyurea, and reduced products of DMF (CO and NHMe2), which also prevent the negative electrode from self-discharge by mitigating the parasitic reaction of dissolved oxygen in the electrolyte. Moreover, a full cell assembled by integrating S@CoWO4 anode and Na0.44MnO2 cathode showed remarkable stability and a high energy density of 119 Wh kg-1, making it a promising candidate for a future energy storage system. Figure 1
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Kang, Hyeonmuk, Taehee Kim, GyuSeong Hwang, GeunHyeong Shin, Junho Lee, and EunAe Cho. "Sustained Release of AgNO3 Additive in Carbonate Electrolytes for Stable Lithium Metal Anodes." ECS Meeting Abstracts MA2022-01, no. 4 (July 7, 2022): 526. http://dx.doi.org/10.1149/ma2022-014526mtgabs.
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With increasing energy storage demand, research on high energy density and stable battery became essential. Among different anode materials for lithium batteries, lithium metal is an ideal anode material as it has low redox potential and high specific capacity. Therefore, for post-lithium ion battery with high energy density cannot avoid using lithium metal as an anode. However, lithium metal anode has stability and safety issues due to dendritic growth. Lithium metal in contact with organic electrolyte reacts with the electrolyte to form solid electrolyte interface (SEI). SEI prevents further electrolyte consumption, however presence of unstable SEI causes uneven lithium ion diffusion through the SEI layer and induces lithium dendrite growth. Therefore, uniform deposition of lithium and stable SEI is important to operate lithium metal anode safely. The application of nitrate additives in carbonate electrolyte has been very limited due to poor solubility. However, nitrate containing polymer interlayer can release additive constantly enabling nitrate act as an electrolyte additive. Herein, AgNO3 synthesized with PAN nanofibers (AgPAN) is used as an additive to induce uniform lithium deposition and stable SEI formation. In the symmetric cell test, life time of 20 µm thick lithium foil enhanced from 140 hr to 300 hr with AgPAN. Lithium nucleation overpotential disappeared and overall overpotential is reduced. Originally, plane lithium foil had the sparsely deposited dendrite shaped lithium, but with AgPAN lithium was evenly deposited and grow in spherical shape. Ag+ reduces on lithium metal surface acting as a lithium nucleation seed helping uniform lithium deposition and NO3 - reacts with lithium to form stable inorganic SEI layer (Li2O, Li3N, LiNxOy, and etc) resulting in stable cycling of lithium metal anode.
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Guo, Juchen. "(Invited) Designing Interphase in Rechargeable Lithium Metal Batteries Via Liquid Electrolyte Additives." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 197. http://dx.doi.org/10.1149/ma2022-012197mtgabs.
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The goal of reaching specific energy at 500 Wh kg-1 resurrects Li metal anode in recent years due to its high capacity (3860 mAh g-1) and low reductive potential (-3.04 V vs. standard hydrogen electrode). However, the reductive decomposition and chemical instability of the liquid electrolytes against Li metal result to unstable solid-electrolyte interphase (SEI) formation and porous Li deposition with low coulombic efficiency and severe volume expansion. Therefore, one strategy to enhance the cycle life of Li metal anode is to design robust SEI to improve the interfacial stability. Herein, we demonstrate two liquid electrolyte additives that can form and regulate desirable SEI on the Li metal anode. Acrylonitrile (AN) can be electrochemically polymerized as an additive to form a Li-ion conductive SEI during Li deposition. Electrochemical analyses, scanning electron microscopy, and X-ray photoelectron spectroscopy confirm the formation of the polymeric SEI, which induces uniform and dense Li deposition and reduced decomposition of the Li-ion electrolyte. Phosphorous pentoxide (P2O5) is also studied as an additive in the typical 1M LiPF6 electrolyte in carbonate solvents for Li metal batteries. P2O5 can effectively scavenges the active impurities in the carbonate electrolytes and form phosphorous-rich stable SEI. Significantly improved battery performance due to these two additives is demonstrated in 0.4 Ah pouch cells composed of LiNi0.6Mn0.2Co0.2O2 (NMC622) cathode (3 mAh cm-2) and Li anode (50 mm thick) with a lean electrolyte/capacity ratio of 3 g/Ah.
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del Olmo, Diego, Maria Elzaurdi, Giorgio Baraldi, Maria Echeverria, and Elixabete Ayerbe. "Unraveling the Interplay between Degradation Mechanisms during Battery Cycling Conditions: Influence on SEI Growth." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 241. http://dx.doi.org/10.1149/ma2023-022241mtgabs.
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Although the solid electrolyte interphase (SEI) is integral for the operation and stability of Li-ion batteries, its continuous growth over the battery life leads to in loss of cyclable material and overall degradation which results in capacity face. Therefore, a proper understanding of the mechanisms and factors involved in the SEI evolution during battery operation is integral for both reliable ageing models, allowing proper prognosis of the state of health (SoH), and improvement of battery lifetime. Generally, studies of SEI growth have focused on calendar ageing experiments, in which the battery is left undisturbed for long periods of time and periodic check-up cycles are performed to estimate the capacity loss over time. Despite significant advances in the understanding of SEI formation with this kind of experiments, the specific limiting mechanism for SEI growth is still under discussion, with electron or Li-interstitial diffusion through the SEI being the main candidates in recent studies. Calendar ageing provides a suitable framework to study SEI growth in almost isolation from other degradation mechanisms but neglects the synergistic effects that can occur between them in real operation conditions, in which the SEI growth will be influenced by other degradation processes. For example, it has been reported that lithium plating can favor SEI formation and that new SEI will growth in exposed active material through cracks in the particles or in the existing SEI. Although initial efforts towards accounting for these synergies are already present in the literature, they have been applied to sparse sets of data and particularized for single chemistries. In this work we focus on the study SEI growth during cell operation and its interplay with other degradation mechanisms in the cell in different regimes to partially isolate degradation processes (e.g., varying cut-off voltages to favor lithium plating). To this end, we carry out electrochemical cycling tests with LNO/Gr and NMC811/Gr full coin cells and also assemble 3-electrode cells to differentiate between positive and negative electrode contributions. Moreover, the individual contributions from the different degradation mechanisms are assessed by combining EIS measurements, incremental capacity analysis and morphological characterization. The results of the characterization are then used to parametrize the implementation of degradation models (SEI, particle cracking, lithium plating, loss of active material...), with both semi-empirical and physics-based approaches, within a Doyle-Fuller-Newman pseudo-2D framework. The results of the model are then compared with the full coin cells experiments and used to evaluate the degradation synergies and provide best-practice approaches to balance battery performance and lifetime. Moreover, the flexibility of the model with degradation is tested using larger publicly available and literature datasets for different chemistries to assess its suitability in cases for which the complete model parameterization is not available (as it is often the case in commercial cells).
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Zhao, Yunhao, Yueyue Wang, Rui Liang, Guobin Zhu, Weixing Xiong, and Honghe Zheng. "Building Polymeric Framework Layer for Stable Solid Electrolyte Interphase on Natural Graphite Anode." Molecules 27, no. 22 (November 13, 2022): 7827. http://dx.doi.org/10.3390/molecules27227827.
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The overall electrochemical performance of natural graphite is intimately associated with the solid electrolyte interphase (SEI) layer developed on its surface. To suppress the interfacial electrolyte decomposition reactions and the high irreversible capacity loss relating to the SEI formation on a natural graphite (NG) surface, we propose a new design of the artificial SEI by the functional molecular cross-linking framework layer, which was synthesized by grafting acrylic acid (AA) and N,N′−methylenebisacrylamide (MBAA) via an in situ polymerization reaction. The functional polymeric framework constructs a robust covalent bonding onto the NG surface with —COOH and facilitates Li+ conduction owing to the effect of the —CONH group, contributing to forming an SEI layer of excellent stability, flexibility, and compactness. From all the benefits, the initial coulombic efficiency, rate performance, and cycling performance of the graphite anode are remarkably improved. In addition, the full cell using the LiNi0.5Co0.2Mn0.3O2 cathode against the modified NG anode exhibits much-prolonged cycle life with a capacity retention of 82.75% after 500 cycles, significantly higher than the cell using the pristine NG anode. The mechanisms relating to the artificial SEI growth on the graphite surface were analyzed. This strategy provides an efficient and feasible approach to the surface optimization for the NG anode in LIBs.
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Chen, Yue-Sheng, and Yu-Sheng Su. "Lithium Silicates as an Artificial SEI for Rechargeable Lithium Metal Batteries." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 680. http://dx.doi.org/10.1149/ma2023-024680mtgabs.
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The major motivation of replacing lithium-ion batteries with lithium metal batteries is to obtain higher energy density by adopting the metallic lithium anode (3860 mAh g-1, theoretically), which means they can store more energy in the same volume or weight. One of the main challenges of rechargeable lithium metal batteries is the formation of lithium dendrites during the charging process.1 Lithium dendrites are tiny needle-like structures that can grow from the surface of the lithium metal electrode and penetrate the separator, causing battery short-circuiting. This can lead to safety issues, including the potential for fire or explosion. Another challenge is the formation of solid-electrolyte interface (SEI) on the surface of the lithium metal electrode, which can reduce the battery's efficiency and cycle life.2 The SEI layer can also lead to the formation of inactive lithium and increase the risk of dendrite growth. In the present work, various lithium silicates have been synthesized to be implemented as the artificial SEI layer via a facile dry coating method.3,4 The lithium silicate coating acts as a protective barrier that prevents direct contact between the lithium metal and the electrolyte, which may cause undesirable side reactions and reduce the efficiency and lifespan of the battery.4 The lithium silicate-based artificial SEI layer improves the stability and efficiency of lithium metal batteries by reducing unwanted surface reactions, improving ion transport kinetics, and protecting the lithium metal anode from mechanical deformation and unstable SEI formation during extended cycling. This laminated lithium anode structure could be an effective design for the future development of long-cycle-life lithium metal batteries. F. Wu et al., Energy Storage Materials, 15, 148–170 (2018). X.-B. Cheng et al., Adv. Sci., 3, 1500213 (2016). A. Bhat, P. Sireesha, Y. Chen, and Y. Su, ChemElectroChem, 9 (2022) https://onlinelibrary.wiley.com/doi/10.1002/celc.202200772. Y.-S. Su, K.-C. Hsiao, P. Sireesha, and J.-Y. Huang, Batteries, 8, 2 (2022). Figure 1
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Kim, Jeongmin, Taeho Yoon, and Oh B. Chae. "Behavior of NO3−-Based Electrolytes Additive in Lithium Metal Batteries." Batteries 10, no. 4 (April 17, 2024): 135. http://dx.doi.org/10.3390/batteries10040135.
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While lithium metal is highly desired as a next-generation battery material due to its theoretically highest capacity and lowest electrode potential, its practical application has been impeded by stability issues such as dendrite formation and short cycle life. Ongoing research aims to enhance the stability of lithium metal batteries for commercialization. Among the studies, research on N-based electrolyte additives, which can stabilize the solid electrolyte interface (SEI) layer and provide stability to the lithium metal surface, holds great promise. The NO3− anion in the N-based electrolyte additive causes the SEI layer on the lithium metal surface to contain compounds such as Li3N and Li2O, which not only facilitates the conduction of Li+ ions in the SEI layer but also increases its mechanical strength. However, due to challenges with the solubility of N-based electrolyte additives in carbonate-based electrolytes, extensive research has been conducted on electrolytes based on ethers. Nonetheless, the low oxidative stability of ether-based electrolytes hinders their practical application. Hence, a strategy is needed to incorporate N-based electrolyte additives into carbonate-based electrolytes. In this review, we address the challenges of lithium metal batteries and propose practical approaches for the application and development of N-based electrolyte additives.
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Ma, Yue, Feng Wu, Nan Chen, Tianyu Yang, Yaohui Liang, Zhaoyang Sun, Guangqiu Luo, et al. "A Dual Functional Artificial SEI Layer Based on a Facile Surface Chemistry for Stable Lithium Metal Anode." Molecules 27, no. 16 (August 15, 2022): 5199. http://dx.doi.org/10.3390/molecules27165199.
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Solid electrolyte interphase (SEI) on a Li anode is critical to the interface stability and cycle life of Li metal batteries. On the one hand, components of SEI with the passivation effect can effectively hinder the interfacial side reactions to promote long-term cycling stability. On the other hand, SEI species that exhibit the active site effect can reduce the Li nucleation barrier and guide Li deposition homogeneously. However, strategies that only focus on a separated effect make it difficult to realize an ideal overall performance of a Li anode. Herein, a dual functional artificial SEI layer simultaneously combining the passivation effect and the active site effect is proposed and constructed via a facial surface chemistry method. Simultaneously, the formed LiF component effectively passivates the anode/electrolyte interface and contributes to the long-term stable cycling performance, while the Li-Mg solid solution alloy with the active site effect promotes the transmission of Li+ and guides homogeneous Li deposition with a low energy barrier. Benefiting from these advantages, the Li||Li cell with the modified anode performs with a lower nucleation overpotential of 2.3 mV, and an ultralong cycling lifetime of over 2000 h at the current density of 1 mA cm−2, while the Li||LiFePO4 full battery maintains a capacity retention of 84.6% at rate of 1 C after 300 cycles.
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Wang, Xinyu, Xiaomin Li, Huiqing Fan, and Longtao Ma. "Solid Electrolyte Interface in Zn-Based Battery Systems." Nano-Micro Letters 14, no. 1 (October 19, 2022). http://dx.doi.org/10.1007/s40820-022-00939-w.
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AbstractDue to its high theoretical capacity (820 mAh g−1), low standard electrode potential (− 0.76 V vs. SHE), excellent stability in aqueous solutions, low cost, environmental friendliness and intrinsically high safety, zinc (Zn)-based batteries have attracted much attention in developing new energy storage devices. In Zn battery system, the battery performance is significantly affected by the solid electrolyte interface (SEI), which is controlled by electrode and electrolyte, and attracts dendrite growth, electrochemical stability window range, metallic Zn anode corrosion and passivation, and electrolyte mutations. Therefore, the design of SEI is decisive for the overall performance of Zn battery systems. This paper summarizes the formation mechanism, the types and characteristics, and the characterization techniques associated with SEI. Meanwhile, we analyze the influence of SEI on battery performance, and put forward the design strategies of SEI. Finally, the future research of SEI in Zn battery system is prospected to seize the nature of SEI, improve the battery performance and promote the large-scale application.
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Jiang, Chunlei, Jiaxiao Yan, Doufeng Wang, Kunye Yan, Lei Shi, Yongping Zheng, Chengde Xie, Hui-Ming Cheng, and Yongbing Tang. "Significant Strain Dissipation via Stiff‐Tough Solid Electrolyte Interphase Design for Highly Stable Alloying Anodes." Angewandte Chemie, October 26, 2023. http://dx.doi.org/10.1002/ange.202314509.
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The pulverization of alloying anodes significantly restricts their use in lithium‐ion batteries (LIBs). This study presents a dual‐phase solid electrolyte interphase (SEI) design that incorporates finely dispersed Al nanoparticles within the LiPON matrix. This distinctive dual‐phase structure imparts high stiffness and toughness to the integrated SEI film. In comparison to single‐phase LiPON film, the optimized Al/LiPON dual‐phase SEI film demonstrates a remarkable increase in fracture toughness by 317.8%, while maintaining stiffness, achieved through the substantial dissipation of strain energy. Application of the dual‐phase SEI film on an Al anode leads to a 450% enhancement in cycling stability for lithium storage in dual‐ion batteries. A similar enhancement in cycling stability for silicon anodes, which face severe volume expansion issues, is also observed, demonstrating the broad applicability of the dual‐phase SEI design. Specifically, homogeneous Li‐Al alloying has been observed in conventional LIBs, even when paired with a high mass loading LiNi0.5Co0.3Mn0.2O2 cathode (7 mg cm–2). The dual‐phase SEI film design can also accelerate the diffusion kinetics of Li‐ions through interface electronic structure regulation. This dual‐phase design can integrate stiffness and toughness into a single SEI film, providing a pathway to enhance both the structural stability and rate capability of alloying anodes.
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Jiang, Chunlei, Jiaxiao Yan, Doufeng Wang, Kunye Yan, Lei Shi, Yongping Zheng, Chengde Xie, Hui-Ming Cheng, and Yongbing Tang. "Significant Strain Dissipation via Stiff‐Tough Solid Electrolyte Interphase Design for Highly Stable Alloying Anodes." Angewandte Chemie International Edition, October 26, 2023. http://dx.doi.org/10.1002/anie.202314509.
Full textAbstract:
The pulverization of alloying anodes significantly restricts their use in lithium‐ion batteries (LIBs). This study presents a dual‐phase solid electrolyte interphase (SEI) design that incorporates finely dispersed Al nanoparticles within the LiPON matrix. This distinctive dual‐phase structure imparts high stiffness and toughness to the integrated SEI film. In comparison to single‐phase LiPON film, the optimized Al/LiPON dual‐phase SEI film demonstrates a remarkable increase in fracture toughness by 317.8%, while maintaining stiffness, achieved through the substantial dissipation of strain energy. Application of the dual‐phase SEI film on an Al anode leads to a 450% enhancement in cycling stability for lithium storage in dual‐ion batteries. A similar enhancement in cycling stability for silicon anodes, which face severe volume expansion issues, is also observed, demonstrating the broad applicability of the dual‐phase SEI design. Specifically, homogeneous Li‐Al alloying has been observed in conventional LIBs, even when paired with a high mass loading LiNi0.5Co0.3Mn0.2O2 cathode (7 mg cm–2). The dual‐phase SEI film design can also accelerate the diffusion kinetics of Li‐ions through interface electronic structure regulation. This dual‐phase design can integrate stiffness and toughness into a single SEI film, providing a pathway to enhance both the structural stability and rate capability of alloying anodes.
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Tripathi, Rashmi, Göktug Yesilbas, Xaver Lamprecht, Pranay Gandharapu, Aliaksandr Bandarenka, Rajiv O. Dusane, and Amartya Mukhopadhyay. "Understanding the Electrolyte Chemistry Induced Enhanced Stability of Si Anodes in Li-Ion Batteries based on Physico-Chemical Changes, Impedance, and Stress Evolution during SEI Formation." Journal of The Electrochemical Society, September 19, 2023. http://dx.doi.org/10.1149/1945-7111/acfb3f.
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Abstract Volume expansion/contraction of Si-based anodes during electrochemical lithiation/delithiation cycles causes loss in mechanical integrity and accrued instability of the solid electrolyte interphase (SEI) layer, culminating into capacity fade. Electrolyte additives like fluoroethylene carbonate (FEC) improve SEI stability, but the associated causes remain under debate. This work reveals some of the roles of FEC via post-mortem observations/analyses, operando stress measurements, and a comprehensive study of the impedance associated with the formation/evolution of SEI during lithiation/delithiation. Usage of 10 vol.% FEC as electrolyte additive leads to significant improvements in cyclic stability and Coulombic efficiency and facilitates smoother/compact/crack-free surface/SEI, in contrast to the cracked/pitted/uneven surface upon non-usage of FEC. Operando stress measurements during SEI formation reveal compressive stress development, followed by loss in mechanical integrity, upon non-usage of electrolyte additive, in contrast to insignificant stress development associated with SEI formation upon usage of FEC. The proposed electrochemical impedance spectroscopy model facilitates good fit with the impedance data at all states-of-charge, with the SEI resistance and capacitance exhibiting expected variations with cycling and the SEI resistance progressively decreasing with cycle number in the presence of FEC. By contrast, in the absence of FEC, severe fluctuations observed with the SEI resistance and capacitance indicate instability.