Unlocking the Power of Lewis Basicity in Oxide Lattice Oxygens: A Regulating Force for Enhanced Oxygen Evolution Kinetics in Li-O2 Batteries.

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Hao-Min Guan,Zhi-Peng Cai,Xue-Yan Wu,Kai-Xue Wang,Jie-Sheng Chen
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引用次数: 0

Abstract

Lithium-oxygen batteries (LOBs) require fast oxygen conversion kinetics to achieve good cycling performance and high energy efficiency. In the text of catalysts for LOBs, Lewis basicity of lattice oxygens (OL) in common transition metal oxides is often underestimated due to the weak electron donor characteristic of OL. In this work, a new spinel-type high entropy oxide with Lewis basicity (LB-HEO) was synthesized through a Joule-heating method. OL was activated by regulating the tetrahedral site-OL-octahedral site (MTd-OL-MOh) units in the spinel-type HEO, enhancing the Lewis basicity. Used as cathode catalyst for LOBs, LB-HEO could attract Li+ and increase the disorder in discharge product, lithium peroxide (Li2O2), promoting the delithiation process and the interfacial charge transfer at the LB-HEO|Li2O2 interface. The activation energy of interfacial charge transfer was significantly reduced from 63.5 kJ mol-1 to 22.4 kJ mol-1. As a result, low charging overpotential of 0.97 V and long cycling lifespan of 135 cycles at 100 mA g-1 were achieved with capacity limitation of 1000 mAh g-1. The strategy based on the regulation of Li+ behavior through its interaction with Lewis bases provides a promising prospective for the design of non-noble metal catalysts for high-performance LOBs.
解锁氧化晶格氧中的路易斯碱度的力量:Li-O2电池中增强的析氧动力学的调节力。
锂氧电池(lob)需要快速的氧转化动力学才能达到良好的循环性能和高能效。在lob催化剂的文献中,由于晶格氧(OL)的弱电子供体特性,通常会低估其在常见过渡金属氧化物中的路易斯碱度。本文采用焦耳加热法合成了一种新型尖晶石型路易斯碱度高熵氧化物(LB-HEO)。OL是通过调节尖晶石型HEO中的四面体-OL-八面体位点(MTd-OL-MOh)来激活的,增强了Lewis碱度。LB-HEO作为lob的阴极催化剂,会吸引Li+,增加放电产物过氧化锂(Li2O2)的无序性,促进LB-HEO|Li2O2界面的氧化过程和界面电荷转移。界面电荷转移活化能从63.5 kJ mol-1降低到22.4 kJ mol-1。在100ma g-1条件下实现了0.97 V的低充电过电位和135次的长循环寿命,容量限制为1000 mAh g-1。基于Li+与Lewis碱相互作用调控Li+行为的策略为设计高性能lob的非贵金属催化剂提供了广阔的前景。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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