Visualization of electrochemically driven solid-state phase transformations using operando hard X-ray spectro-imaging

Linsen Li, Yu-chen Karen Chen-Wiegart, Jiajun Wang, Peng Gao, Qi Ding, Young-Sang Yu, Feng Wang, Jordi Cabana, Jun Wang and Song Jin ()
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Linsen Li: University of Wisconsin—Madison
Yu-chen Karen Chen-Wiegart: Photon Sciences Directorate, Brookhaven National Laboratory
Jiajun Wang: Photon Sciences Directorate, Brookhaven National Laboratory
Peng Gao: Brookhaven National Laboratory
Qi Ding: University of Wisconsin—Madison
Young-Sang Yu: Advanced Light Source, Lawrence Berkeley National Laboratory
Feng Wang: Brookhaven National Laboratory
Jordi Cabana: University of Illinois at Chicago
Jun Wang: Photon Sciences Directorate, Brookhaven National Laboratory
Song Jin: University of Wisconsin—Madison

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract In situ techniques with high temporal, spatial and chemical resolution are key to understand ubiquitous solid-state phase transformations, which are crucial to many technological applications. Hard X-ray spectro-imaging can visualize electrochemically driven phase transformations but demands considerably large samples with strong absorption signal so far. Here we show a conceptually new data analysis method to enable operando visualization of mechanistically relevant weakly absorbing samples at the nanoscale and study electrochemical reaction dynamics of iron fluoride, a promising high-capacity conversion cathode material. In two specially designed samples with distinctive microstructure and porosity, we observe homogeneous phase transformations during both discharge and charge, faster and more complete Li-storage occurring in porous polycrystalline iron fluoride, and further, incomplete charge reaction following a pathway different from conventional belief. These mechanistic insights provide guidelines for designing better conversion cathode materials to realize the promise of high-capacity lithium-ion batteries.

Date: 2015
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DOI: 10.1038/ncomms7883

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