过电位
电负性
路易斯酸
阴极
无机化学
氧气
密度泛函理论
析氧
化学
物理化学
电化学
电极
计算化学
催化作用
有机化学
作者
Yin Zhou,Kun Yin,Qianfeng Gu,Lu Tao,Yiju Li,Hao Tan,Jinhui Zhou,Wenshu Zhang,Hongbo Li,Shaojun Guo
标识
DOI:10.1002/ange.202114067
摘要
Abstract The sluggish oxygen reaction kinetics concomitant with the high overpotentials and parasitic reactions from cathodes and solvents is the major challenge in aprotic lithium‐oxygen (Li–O 2 ) batteries. Herein, PtIr multipods with a low Lewis acidity of the Pt atoms are reported as an advanced cathode for improving overpotentials and stabilities. DFT calculations disclose that electrons have a strong disposition to transfer from Ir to Pt, since Pt has a higher electronegativity than Ir, resulting in a lower Lewis acidity of the Pt atoms than that on the pure Pt surface. The low Lewis acidity of Pt atoms on the PtIr surface entails a high electron density and a down‐shifting of the d‐band center, thereby weakening the binding energy towards intermediates (LiO 2 ), which is the key in achieving low oxygen‐reduction‐reaction (ORR) and oxygen‐evolution‐reaction (OER) overpotentials. The Li–O 2 cell based on PtIr electrodes exhibits a very low overall discharge/charge overpotential (0.44 V) and an excellent cycle life (180 cycles), outperforming the bulk of reported noble‐metal‐based cathodes.
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