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 -