In situ and operando investigation of the dynamic morphological and phase changes of a selenium-doped germanium electrode during (de)lithiation processes

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

doi:10.1039/c9ta09750c

Title: In situ and operando investigation of the dynamic morphological and phase changes of a selenium-doped germanium electrode during (de)lithiation processes

Journal Article · 05 December 2019 · Journal of Materials Chemistry. A

DOI: https://doi.org/10.1039/c9ta09750c · OSTI ID:1798830

^[1]; Lim, Cheolwoong ^[1]; Cui, Yi ^[1]; Zhou, Xinwei ^[2]; Kang, Huixiao ^[1]; Yan, Bo ^[3]; Meyerson, Melissa L. ^[4]; Weeks, Jason A. ^[4]; Liu, Qi ^[5]; Guo, Fangmin ^[5]; Kou, Ronghui ^[5]; Liu, Yuzi ^[5]; De Andrade, Vincent ^[5]; De Carlo, Francesco ^[5]; Ren, Yang ^[5]; Sun, Cheng-Jun ^[5];

^[4]; Chen, Lei ^[6];

^[7];

^[1]

Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Shanghai Jiao Tong Univ. (China)
Univ. of Texas, Austin, TX (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Mississippi State Univ., Mississippi State, MS (United States)
Zhengzhou Univ. (China)

To understand the effect of selenium doping on the good cycling performance and rate capability of a Ge_0.9Se_0.1 electrode, the dynamic morphological and phase changes of the Ge_0.9Se_0.1 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 Ge_0.9Se_0.1 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 Ge_0.9Se_0.1 and Ge is attributed to a super-ionically conductive Li–Se–Ge network formed inside Ge_0.9Se_0.1 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. Finally, 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); Robert A. Welch Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1798830

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 2 Vol. 8; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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