Shengqin Guan, Baoen Xu, Xingbo Yu, Yonghong Ye, Yuting Liu, Taotao Guan, Yu Yang, Jiali Gao, Kaixi Li, Jianlong Wang
{"title":"在掺氮高熵氧化物纳米片中激活晶格氧,实现高效氧气进化反应","authors":"Shengqin Guan, Baoen Xu, Xingbo Yu, Yonghong Ye, Yuting Liu, Taotao Guan, Yu Yang, Jiali Gao, Kaixi Li, Jianlong Wang","doi":"10.1021/acscatal.4c05997","DOIUrl":null,"url":null,"abstract":"High-entropy oxides (HEOs) are potential electrocatalysts for overcoming the sluggish kinetics of the oxygen evolution reaction (OER). Conventionally, the thermodynamic barrier of the lattice oxygen mechanism (LOM) is lower than that of the adsorbate evolution mechanism (AEM). However, controlling the transition from the AEM to the LOM remains challenging. Herein, an in situ modulation strategy has been developed to synthesize N-FeCoNiAlMoO<sub><i>x</i></sub> by introducing structural directing agents and electronic modulators. Different instruments were used to identify the nitridation-triggered micromorphologies and phase transformations. X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure spectroscopy (XAFS) reveal the optimized electronic structures after nitrogen doping. N-FeCoNiAlMo<sub><i>x</i></sub> exhibits OER performance with low overpotentials of 240 and 285 mV at 10 and 100 mA·cm<sup>–2</sup>, respectively. pH dependence, free-radical capture experiments, and density functional theory (DFT) calculations confirm that nitrogen doping facilitates the LOM pathway. This work elucidates nitrogen’s critical role and the LOM pathway’s contribution to efficient OER performance.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"9 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Activation of Lattice Oxygen in Nitrogen-Doped High-Entropy Oxide Nanosheets for Highly Efficient Oxygen Evolution Reaction\",\"authors\":\"Shengqin Guan, Baoen Xu, Xingbo Yu, Yonghong Ye, Yuting Liu, Taotao Guan, Yu Yang, Jiali Gao, Kaixi Li, Jianlong Wang\",\"doi\":\"10.1021/acscatal.4c05997\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"High-entropy oxides (HEOs) are potential electrocatalysts for overcoming the sluggish kinetics of the oxygen evolution reaction (OER). Conventionally, the thermodynamic barrier of the lattice oxygen mechanism (LOM) is lower than that of the adsorbate evolution mechanism (AEM). However, controlling the transition from the AEM to the LOM remains challenging. Herein, an in situ modulation strategy has been developed to synthesize N-FeCoNiAlMoO<sub><i>x</i></sub> by introducing structural directing agents and electronic modulators. Different instruments were used to identify the nitridation-triggered micromorphologies and phase transformations. X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure spectroscopy (XAFS) reveal the optimized electronic structures after nitrogen doping. N-FeCoNiAlMo<sub><i>x</i></sub> exhibits OER performance with low overpotentials of 240 and 285 mV at 10 and 100 mA·cm<sup>–2</sup>, respectively. pH dependence, free-radical capture experiments, and density functional theory (DFT) calculations confirm that nitrogen doping facilitates the LOM pathway. This work elucidates nitrogen’s critical role and the LOM pathway’s contribution to efficient OER performance.\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"9 1\",\"pages\":\"\"},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2024-11-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acscatal.4c05997\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c05997","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Activation of Lattice Oxygen in Nitrogen-Doped High-Entropy Oxide Nanosheets for Highly Efficient Oxygen Evolution Reaction
High-entropy oxides (HEOs) are potential electrocatalysts for overcoming the sluggish kinetics of the oxygen evolution reaction (OER). Conventionally, the thermodynamic barrier of the lattice oxygen mechanism (LOM) is lower than that of the adsorbate evolution mechanism (AEM). However, controlling the transition from the AEM to the LOM remains challenging. Herein, an in situ modulation strategy has been developed to synthesize N-FeCoNiAlMoOx by introducing structural directing agents and electronic modulators. Different instruments were used to identify the nitridation-triggered micromorphologies and phase transformations. X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure spectroscopy (XAFS) reveal the optimized electronic structures after nitrogen doping. N-FeCoNiAlMox exhibits OER performance with low overpotentials of 240 and 285 mV at 10 and 100 mA·cm–2, respectively. pH dependence, free-radical capture experiments, and density functional theory (DFT) calculations confirm that nitrogen doping facilitates the LOM pathway. This work elucidates nitrogen’s critical role and the LOM pathway’s contribution to efficient OER performance.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.