{"title":"Effect of A-Site Defects on the Catalytic Activity of Perovskite LaCoO3: Insights from the Electronic Structure","authors":"Hanlin Chen, Xiaoliang Liang, Zijuan You, Fuding Tan, Jingwen Zhou, Xiaoju Lin, Meiqin Chen, Peng Liu, Yiping Yang, Suhua Wang, Steven L. Suib","doi":"10.1021/acscatal.4c06142","DOIUrl":null,"url":null,"abstract":"The development of highly active perovskite-based catalysts for the oxidation of volatile organic chemicals (VOCs) has drawn a great deal of attention. A-site defect regulation is found to be effective to improve the catalytic performance, but the relationship between structure variation and catalytic activity has not been clearly unveiled. Herein, this issue was interpreted by the variation of physicochemical properties and electronic structure (O p-band center). An <i>in situ</i> one-step calcination method with NH<sub>4</sub>HCO<sub>3</sub> addition was adopted to prepare a series of A-site-deficient LaCoO<sub>3</sub> perovskites (L<sub><i>x</i></sub>CO), which were characterized by XRD, TEM, EELS, ESR, XPS, UPS, H<sub>2</sub>-TPR, and O<sub>2</sub>-TPD and catalytic test toward toluene oxidation. The catalytic activity displayed a volcano-type relationship with an addition amount of NH<sub>4</sub>HCO<sub>3</sub>. The electronic structure determined the reducibility and active oxygen content and accordingly affected the catalytic activity of L<sub><i>x</i></sub>CO. The obtained results provide theoretical and technical support for the design of efficient VOC oxidation catalysts.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"55 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2025-01-17","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.4c06142","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The development of highly active perovskite-based catalysts for the oxidation of volatile organic chemicals (VOCs) has drawn a great deal of attention. A-site defect regulation is found to be effective to improve the catalytic performance, but the relationship between structure variation and catalytic activity has not been clearly unveiled. Herein, this issue was interpreted by the variation of physicochemical properties and electronic structure (O p-band center). An in situ one-step calcination method with NH4HCO3 addition was adopted to prepare a series of A-site-deficient LaCoO3 perovskites (LxCO), which were characterized by XRD, TEM, EELS, ESR, XPS, UPS, H2-TPR, and O2-TPD and catalytic test toward toluene oxidation. The catalytic activity displayed a volcano-type relationship with an addition amount of NH4HCO3. The electronic structure determined the reducibility and active oxygen content and accordingly affected the catalytic activity of LxCO. The obtained results provide theoretical and technical support for the design of efficient VOC oxidation catalysts.
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.