{"title":"Unlocking the Power of Lewis Basicity in Oxide Lattice Oxygens: A Regulating Force for Enhanced Oxygen Evolution Kinetics in Li-O2 Batteries.","authors":"Hao-Min Guan,Zhi-Peng Cai,Xue-Yan Wu,Kai-Xue Wang,Jie-Sheng Chen","doi":"10.1002/anie.202509132","DOIUrl":null,"url":null,"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.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"273 1","pages":"e202509132"},"PeriodicalIF":16.1000,"publicationDate":"2025-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202509132","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
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.
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.