期刊
NANO LETTERS
卷 15, 期 5, 页码 3309-3316出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.5b00521
关键词
in situ NMR; Li-S batteries; radicals; energy storage
类别
资金
- Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences (BES)
- DOE's Office of Biological and Environmental Research (BER)
- PNNL
- U.S. Army Corps of Engineers, Portland District
- Department of Energy [DE-AC05-76RLO1830]
A fundamental understanding of electrochemical reaction pathways is critical to improving the performance of Li-S batteries, but few techniques can be used to directly identify and quantify the reaction species during disharge/charge cycling processes in real time. Here, an in situ Li-7 NMR technique employing a specially designed cylindrical microbattery was used to probe the transient electrochemical and chemical reactions occurring during the cycling of a Li-S system. In situ NMR provides real time, semiquantitative information related to the temporal evolution of lithium polysulfide allotropes during both discharge/charge processes. This technique uniquely reveals that the polysulfide redox reactions involve charged free radicals as intermediate species that are difficult to detect in ex situ NMR studies. Additionally, it also uncovers vital information about the Li-7 chemical environments during the electrochemical and parasitic reactions on the Li metal anode. These new molecular-level insights about transient species and the associated anode failure mechanism are crucial to delineating effective strategies to accelerate the development of Li-S battery technologies.
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