Journal
NATURE COMMUNICATIONS
Volume 6, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms7883
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Funding
- NSF [DMR-1106184]
- UW-Madison WEI Seed Grant
- Research Corporation SciaLog Award
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- Laboratory Directed Research and Development (LDRD) program at Brookhaven National Laboratory
- NorthEast Center for Chemical Energy Storage (NECCES), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012583]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1106184] Funding Source: National Science Foundation
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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.
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