期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 48, 页码 21728-21735出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009528
关键词
mesoporous bismuth; Mg; Bi batteries; Mg(2+)storage mechanism; operando synchrotron; theoretical computations
资金
- Australian Research Council [DP160104866, DE20010124, FL170100154]
- Powder Diffraction and X-ray Absorption Spectroscopy beamlines at the Australian Synchrotron, ANSTO, Melbourne
We present mesoporous bismuth nanosheets as a model to study the charge-storage mechanism of Mg/Bi systems in magnesium-ion batteries (MIBs). Using a systematic spectroscopy investigation of combined synchrotron-based operando X-ray diffraction, near-edge X-ray absorption fine structure and Raman, we demonstrate a reversible two-step alloying reaction mechanism Bi <-> MgBi <-> Mg3Bi2. Ab-initio simulation methods disclose the formation of a MgBi intermediate and confirm its high electronic conductivity. This intermediate serves as a buffer for the significant volume expansion (204 %) and acts to regulate Mg storage kinetics. The mesoporous bismuth nanosheets, as an ideal material for the investigation of the Mg charge-storage mechanism, effectively alleviate volume expansion and enable significant electrochemical performance in a lithium-free electrolyte. These findings will benefit mechanistic understandings and advance material designs for MIBs.
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