TY - JOUR A1 - Xu, Yaolin A1 - Dong, Kang A1 - Jie, Yulin A1 - Adelhelm, Philipp A1 - Chen, Yawei A1 - Xu, Liang A1 - Yu, Peiping A1 - Kim, Junghwa A1 - Kochovski, Zdravko A1 - Yu, Zhilong A1 - Li, Wanxia A1 - LeBeau, James A1 - Shao-Horn, Yang A1 - Cao, Ruiguo A1 - Jiao, Shuhong A1 - Cheng, Tao A1 - Manke, Ingo A1 - Lu, Yan T1 - Promoting mechanistic understanding of lithium deposition and solid-electrolyte interphase (SEI) formation using advanced characterization and simulation methods: recent progress, limitations, and future perspectives JF - Avanced energy materials N2 - In recent years, due to its great promise in boosting the energy density of lithium batteries for future energy storage, research on the Li metal anode, as an alternative to the graphite anode in Li-ion batteries, has gained significant momentum. However, the practical use of Li metal anodes has been plagued by unstable Li (re)deposition and poor cyclability. Although tremendous efforts have been devoted to the stabilization of Li metal anodes, the mechanisms of electrochemical (re-)deposition/dissolution of Li and solid-electrolyte-interphase (SEI) formation remain elusive. This article highlights the recent mechanistic understandings and observations of Li deposition/dissolution and SEI formation achieved from advanced characterization techniques and simulation methods, and discusses major limitations and open questions in these processes. In particular, the authors provide their perspectives on advanced and emerging/potential methods for obtaining new insights into these questions. In addition, they give an outlook into cutting-edge interdisciplinary research topics for Li metal anodes. It pushes beyond the current knowledge and is expected to accelerate development toward a more in-depth and comprehensive understanding, in order to guide future research on Li metal anodes toward practical application. KW - advanced characterization KW - Li deposition KW - Li dissolution KW - Li metal KW - anodes KW - mechanistic understanding KW - solid-electrolyte-interphase KW - theoretical simulation Y1 - 2022 U6 - https://doi.org/10.1002/aenm.202200398 SN - 1614-6832 SN - 1614-6840 VL - 12 IS - 19 PB - Wiley CY - Weinheim ER - TY - JOUR A1 - Sun, Fu A1 - Osenberg, Markus A1 - Dong, Kang A1 - Zhou, Dong A1 - Hilger, Andre A1 - Jafta, Charl J. A1 - Risse, Sebastian A1 - Lu, Yan A1 - Markoetter, Henning A1 - Manke, Ingo T1 - Correlating Morphological Evolution of Li Electrodes with Degrading Electrochemical Performance of Li/LiCoO2 and Li/S Battery Systems BT - Investigated by Synchrotron X-ray Phase Contrast Tomography JF - ACS energy letters / American Chemical Society N2 - Efficient Li utilization is generally considered to be a prerequisite for developing next-generation energy storage systems (ESSs). However, uncontrolled growth of Li microstructures (LmSs) during electrochemical cycling has prevented its practical commercialization. Herein, we attempt to understand the correlation of morphological evolution of Li electrodes with degrading electrochemical performances of Li/LiCoO2 and Li/S systems by synchrotron X-ray phase contrast tomography technique. It was found that the continuous transformation of the initial dense Li bulk to a porous lithium interface (PL1) structure intimately correlates with the gradually degrading overall cell performance of these two systems. Additionally, the formation mechanism of the PLI and its correlation with previously reported inwardly growing LmS and the lithium-reacted region have been intensively discussed. The information that we gain herein is complementary to previous investigations and may provide general insights into understanding of degradation mechanisms of Li metal anodes and also provide highly needed guidelines for effective design of reliable next-generation Li metal-based ESSs. Y1 - 2018 U6 - https://doi.org/10.1021/acsenergylett.7b01254 SN - 2380-8195 VL - 3 IS - 2 SP - 356 EP - 365 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Sun, Fu A1 - Dong, Kang A1 - Osenberg, Markus A1 - Hilger, Andre A1 - Risse, Sebastian A1 - Lu, Yan A1 - Kamm, Paul H. A1 - Klaus, Manuela A1 - Markoetter, Henning A1 - Garcia-Moreno, Francisco A1 - Arlt, Tobias A1 - Manke, Ingo T1 - Visualizing the morphological and compositional evolution of the interface of InLi-anode|thio-LISION electrolyte in an all-solid-state Li-S cell by in operando synchrotron X-ray tomography and energy dispersive diffraction JF - Journal of materials chemistry : A, Materials for energy and sustainability N2 - Dynamic and direct visualization of interfacial evolution is helpful in gaining fundamental knowledge of all-solid-state-lithium battery working/degradation mechanisms and clarifying future research directions for constructing next-generation batteries. Herein, in situ and in operando synchrotron X-ray tomography and energy dispersive diffraction were simultaneously employed to record the morphological and compositional evolution of the interface of InLi-anode|sulfide-solid-electrolyte during battery cycling. Compelling morphological evidence of interfacial degradation during all-solid-state-lithium battery operation has been directly visualized by tomographic measurement. The accompanying energy dispersive diffraction results agree well with the observed morphological deterioration and the recorded electrochemical performance. It is concluded from the current investigation that a fundamental understanding of the phenomena occurring at the solid-solid electrode|electrolyte interface during all-solid-state-lithium battery cycling is critical for future progress in cell performance improvement and may determine its final commercial viability. Y1 - 2018 U6 - https://doi.org/10.1039/c8ta08821g SN - 2050-7488 SN - 2050-7496 VL - 6 IS - 45 SP - 22489 EP - 22496 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Ning, Jiaoyi A1 - Yu, Hongtao A1 - Mei, Shilin A1 - Schütze, Yannik A1 - Risse, Sebastian A1 - Kardjilov, Nikolay A1 - Hilger, André A1 - Manke, Ingo A1 - Bande, Annika A1 - Ruiz, Victor G. A1 - Dzubiella, Joachim A1 - Meng, Hong A1 - Lu, Yan T1 - Constructing binder- and carbon additive-free organosulfur cathodes based on conducting thiol-polymers through electropolymerization for lithium-sulfur batteries JF - ChemSusChem N2 - Herein, the concept of constructing binder- and carbon additive-free organosulfur cathode was proved based on thiol-containing conducting polymer poly(4-(thiophene-3-yl) benzenethiol) (PTBT). The PTBT featured the polythiophene-structure main chain as a highly conducting framework and the benzenethiol side chain to copolymerize with sulfur and form a crosslinked organosulfur polymer (namely S/PTBT). Meanwhile, it could be in-situ deposited on the current collector by electro-polymerization, making it a binder-free and free-standing cathode for Li-S batteries. The S/PTBT cathode exhibited a reversible capacity of around 870 mAh g(-1) at 0.1 C and improved cycling performance compared to the physically mixed cathode (namely S&PTBT). This multifunction cathode eliminated the influence of the additives (carbon/binder), making it suitable to be applied as a model electrode for operando analysis. Operando X-ray imaging revealed the remarkable effect in the suppression of polysulfides shuttle via introducing covalent bonds, paving the way for the study of the intrinsic mechanisms in Li-S batteries. KW - electrochemistry KW - energy storage KW - lithium-sulfur batteries KW - operando KW - studies KW - organosulfur Y1 - 2022 U6 - https://doi.org/10.1002/cssc.202200434 SN - 1864-5631 SN - 1864-564X VL - 15 IS - 14 PB - Wiley CY - Weinheim ER -