电位决定非水溶剂锂氧电池的放电机理
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摘要
锂氧电池的放电过程依赖于Li~+参与的氧还原反应(Li~+-ORR),但是目前对Li~+-ORR的机理缺乏深入认识。本文利用现场光谱电化学结合第一性原理,研究了Li~+/DMSO体系的氧还原机理,揭示了O_2~-和LiO_2在Li_2O_2生成过程中的作用,确定了Li~+-ORR中间产物和基元反应,提出了电位相关的溶液相和表面相生成Li_2O_2的反应机理。
Discharging of aprotic Li-O_2 batteries relies on the oxygen reduction reaction(Li~+-ORR),which remains incompletely understood.Herein,we report a mechanistic study of the Li~+-ORR in Li/DMSO.By the spectroelectrochemical identification coupled with density functional theory calculations,we verified the effect of O_2~- and LiO_2 in the process of Li_2O_2 formation.We also confirmed the intermediate product and elementary reactions,and proposed the potential-dependent solution- and surface-mediated pathways for Li_2O_2 formation.
引文
[1]Zhang Y,Zhang X,Wang J,McKee WC,XuY,Peng Z,J.Phys.Chem.C 2016:120,3690-3698.
    [2]Peng Z,S.Freunberger A,Chen Y,Bruce P G,Science,2012:337,563-566.
    [3]Wang J,Zhang Y,Guo L,Wang E,Peng Z.Angew.Chem.,Int.Ed.2016.

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