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Item In Situ and Operando Investigation of the Dynamic Morphological and Phase Changes of Selenium-doped Germanium Electrode during (De)Lithiation Processes(RSC, 2020-01) Li, Tianyi; Lim, Cheolwoong; Cui, Yi; Zhou, Xinwei; Kang, Huixiao; Yan, Bo; Meyerson, Melissa L.; Weeks, Jason A.; Liu, Qi; Guo, Fangmin; Kou, Ronghui; Liu, Yuzi; De Andrade, Vincent; De Carlo, Francesco; Ren, Yang; Sun, Cheng-Jun; Mullins, C. Buddie; Chen, Lei; Fu, Yongzhu; Zhu, Likun; Mechanical and Energy Engineering, School of Engineering and TechnologyTo understand the effect of selenium doping on the good cycling performance and rate capability of a Ge0.9Se0.1 electrode, the dynamic morphological and phase changes of the Ge0.9Se0.1 electrode were investigated by synchrotron-based operando transmission X-ray microscopy (TXM) imaging, X-ray diffraction (XRD), and X-ray absorption spectroscopy (XAS). The TXM results show that the Ge0.9Se0.1 particle retains its original shape after a large volume change induced by (de)lithiation and undergoes a more sudden morphological and optical density change than pure Ge. The difference between Ge0.9Se0.1 and Ge is attributed to a super-ionically conductive Li–Se–Ge network formed inside Ge0.9Se0.1 particles, which contributes to fast Li-ion pathways into the particle and nano-structuring of Ge as well as buffering the volume change of Ge. The XRD and XAS results confirm the formation of a Li–Se–Ge network and reveal that the Li–Se–Ge phase forms during the early stages of lithiation and is an inactive phase. The Li–Se–Ge network also can suppress the formation of the crystalline Li15Ge4 phase. These in situ and operando results reveal the effect of the in situ formed, super-ionically conductive, and inactive network on the cycling performance of Li-ion batteries and shed light on the design of high capacity electrode materials.Item Three-Dimensional Reconstruction and Analysis of All-Solid Li-Ion Battery Electrode Using Synchrotron Transmission X-ray Microscopy Tomography(ACS, 2018-05) Li, Tianyi; Kang, Huixiao; Zhou, Xinwei; Lim, Cheolwoong; Yan, Bo; De Andrade, Vincent; De Carlo, Francesco; Zhu, Likun; Mechanical Engineering, School of Engineering and TechnologyA synchrotron transmission X-ray microscopy tomography system with a spatial resolution of 58.2 nm at the Advanced Photon Source was employed to obtain three-dimensional morphological data of all-solid Li-ion battery electrodes. The three-phase electrode was fabricated from a 47:47:6 (wt %) mixture of Li(Ni1/3Mn1/3Co1/3)O2 as active material, Li1.3Ti1.7Al0.3(PO4)3 as Li-ion conductor, and Super-P carbon as electron conductor. The geometric analysis show that particle-based all-solid Li-ion battery has serious contact interface problem which significantly impact the Li-ion transport and intercalation reaction in the electrode, leading to low capacity, poor rate capability and cycle life.