Ma Shunchao, Wang Jiawei, Huang Jun, Zhou Zhen, Peng Zhangquan
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry , Chinese Academy of Sciences , Changchun , Jilin 130022 , People's Republic of China.
University of Chinese Academy of Sciences , Beijing 100039 , People's Republic of China.
J Phys Chem Lett. 2018 Jun 21;9(12):3333-3339. doi: 10.1021/acs.jpclett.8b01333. Epub 2018 Jun 6.
The addition of HO, even trace amount, in aprotic Li-O batteries has a remarkable impact on achieving high capacity by triggering solution mechanism, and even reducing charge overpotential. However, the critical role of HO in promoting solution mechanism still lacks persuasive spectroscopic evidence, moreover, the origin of low polarization remains incompletely understood. Herein, by in situ spectroscopic identification of reaction intermediates, we directly verify that HO additive is able to alter oxygen reduction reaction (ORR) pathway subjected to solution-mediated growth mechanism of LiO. In addition, ingress of HO also induces to form partial LiOH, resulting in reduced charging polarization due to its higher conductivity; however, LiOH could not contribute to O evolution upon recharge. These original results unveil the complex effects of HO on cycling the aprotic Li-O batteries, which are instructive for the mechanism study of aprotic Li-O batteries with protic additives or soluble catalysts.
在非质子锂氧电池中添加羟基（HO），即使是痕量的，也会通过触发溶解机制对实现高容量产生显著影响，甚至降低充电过电位。然而，羟基在促进溶解机制中的关键作用仍缺乏有说服力的光谱证据，此外，低极化的起源仍未完全理解。在此，通过对反应中间体进行原位光谱鉴定，我们直接验证了羟基添加剂能够改变受LiO溶解介导生长机制影响的氧还原反应（ORR）途径。此外，羟基的进入还诱导形成部分LiOH，由于其较高的电导率导致充电极化降低；然而，LiOH在充电时对析氧没有贡献。这些原始结果揭示了羟基对非质子锂氧电池循环的复杂影响，这对含质子添加剂或可溶性催化剂的非质子锂氧电池的机理研究具有指导意义。
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