@article{SunOsenbergDongetal.2018, author = {Sun, Fu and Osenberg, Markus and Dong, Kang and Zhou, Dong and Hilger, Andre and Jafta, Charl J. and Risse, Sebastian and Lu, Yan and Markoetter, Henning and Manke, Ingo}, title = {Correlating Morphological Evolution of Li Electrodes with Degrading Electrochemical Performance of Li/LiCoO2 and Li/S Battery Systems}, series = {ACS energy letters / American Chemical Society}, volume = {3}, journal = {ACS energy letters / American Chemical Society}, number = {2}, publisher = {American Chemical Society}, address = {Washington}, issn = {2380-8195}, doi = {10.1021/acsenergylett.7b01254}, pages = {356 -- 365}, year = {2018}, abstract = {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.}, language = {en} } @article{SunDongOsenbergetal.2018, author = {Sun, Fu and Dong, Kang and Osenberg, Markus and Hilger, Andre and Risse, Sebastian and Lu, Yan and Kamm, Paul H. and Klaus, Manuela and Markoetter, Henning and Garcia-Moreno, Francisco and Arlt, Tobias and Manke, Ingo}, title = {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}, series = {Journal of materials chemistry : A, Materials for energy and sustainability}, volume = {6}, journal = {Journal of materials chemistry : A, Materials for energy and sustainability}, number = {45}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {2050-7488}, doi = {10.1039/c8ta08821g}, pages = {22489 -- 22496}, year = {2018}, abstract = {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.}, language = {en} } @article{NingYuMeietal.2022, author = {Ning, Jiaoyi and Yu, Hongtao and Mei, Shilin and Sch{\"u}tze, Yannik and Risse, Sebastian and Kardjilov, Nikolay and Hilger, Andr{\´e} and Manke, Ingo and Bande, Annika and Ruiz, Victor G. and Dzubiella, Joachim and Meng, Hong and Lu, Yan}, title = {Constructing binder- and carbon additive-free organosulfur cathodes based on conducting thiol-polymers through electropolymerization for lithium-sulfur batteries}, series = {ChemSusChem}, volume = {15}, journal = {ChemSusChem}, number = {14}, publisher = {Wiley}, address = {Weinheim}, issn = {1864-5631}, doi = {10.1002/cssc.202200434}, pages = {10}, year = {2022}, abstract = {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.}, language = {en} } @article{XuDongJieetal.2022, author = {Xu, Yaolin and Dong, Kang and Jie, Yulin and Adelhelm, Philipp and Chen, Yawei and Xu, Liang and Yu, Peiping and Kim, Junghwa and Kochovski, Zdravko and Yu, Zhilong and Li, Wanxia and LeBeau, James and Shao-Horn, Yang and Cao, Ruiguo and Jiao, Shuhong and Cheng, Tao and Manke, Ingo and Lu, Yan}, title = {Promoting mechanistic understanding of lithium deposition and solid-electrolyte interphase (SEI) formation using advanced characterization and simulation methods: recent progress, limitations, and future perspectives}, series = {Avanced energy materials}, volume = {12}, journal = {Avanced energy materials}, number = {19}, publisher = {Wiley}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.202200398}, pages = {22}, year = {2022}, abstract = {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.}, language = {en} }