期刊
ADVANCED MATERIALS
卷 32, 期 52, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202003879
关键词
potassium– selenium batteries; reaction mechanism; small‐ molecular Se
类别
资金
- National Key R&D Program of China [2018YFB0905400]
- National Natural Science Foundation of China [52002083, 51925207, U1910210, 51872277, 51872283, 2180527]
- Fundamental Research Funds for the Central Universities [WK2060140026]
- National Postdoctoral Program for Innovative Talents [BX20200318]
- China Postdoctoral Science Foundation [2020M682031, 2020M672533]
- Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, CAS [DNL180310, DNL180308, DNL201912, DNL201915]
- Liaoning BaiQianWan Talents Program
- LiaoNing Revitalization Talents Program [XLYC1807153]
- DICP [DICP ZZBS201708, DICP ZZBS201802, DICP I202032]
- U. S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office under US-China clean energy program CERC-CVC2
- DOE Office of Science by UChicago Argonne, LLC [DE-AC02-06CH11357]
The potassium-selenium (K-Se) battery is considered as an alternative solution for stationary energy storage because of abundant resource of K. However, the detailed mechanism of the energy storage process is yet to be unraveled. Herein, the findings in probing the working mechanism of the K-ion storage in Se cathode are reported using both experimental and computational approaches. A flexible K-Se battery is prepared by employing the small-molecule Se embedded in freestanding N -doped porous carbon nanofibers thin film (Se@NPCFs) as cathode. The reaction mechanisms are elucidated by identifying the existence of short-chain molecular Se encapsulated inside the microporous host, which transforms to K2Se by a two-step conversion reaction via an all-solid-state electrochemical process in the carbonate electrolyte system. Through the whole reaction, the generation of polyselenides (K2Sen, 3 <= n <= 8) is effectively suppressed by electrochemical reaction dominated by Se-2 molecules, thus significantly enhancing the utilization of Se and effecting the voltage platform of the K-Se battery. This work offers a practical pathway to optimize the K-Se battery performance through structure engineering and manipulation of selenium chemistry for the formation of selective species and reveal its internal reaction mechanism in the carbonate electrolyte.
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