{"title":"甘油与CO2羰基化反应中CeO2催化剂上氧空位的操纵","authors":"Bowen Tan, Danru Xu, Mengmeng Jin, Bolun Yang, Zhun Hu* and Jingjun Liu*, ","doi":"10.1021/acs.iecr.4c0439210.1021/acs.iecr.4c04392","DOIUrl":null,"url":null,"abstract":"<p >Cerium dioxide (CeO<sub>2</sub>) with different morphologies was synthesized via a hydrothermal method and applied to the carbonylation of glycerol with CO<sub>2</sub>. Subsequent characterization through H<sub>2</sub>-TPR and catalytic activity tests demonstrated that CeO<sub>2</sub> nanorods exhibited the highest oxygen storage/release capacity as well as enhanced catalytic performance compared to other morphologies. CeO<sub>2</sub> nanorods were thus further modified through hydrogen reduction at varying temperatures, aiming to tune the density of the oxygen vacancies. Characterization via BET, NH<sub>3</sub>-TPD, CO<sub>2</sub>-TPD, XPS, and ESR indicated that variations in morphology and reduction temperature influenced the microstructural characteristics and the strength of the acid–base sites of the catalysts. Notably, hydrogen reduction created more oxygen vacancies in the CeO<sub>2</sub> nanorods, with the concentration of these vacancies increasing with higher reduction temperatures. Furthermore, the catalytic activity of CeO<sub>2</sub> in glycerol carbonylation with CO<sub>2</sub> showed a positive correlation with the concentration of oxygen vacancies. Optimizing CeO<sub>2</sub> catalysts can enhance its performance in activating CO<sub>2</sub>, providing new ideas for industrial CO<sub>2</sub> resource utilization and carbon capture technology development.</p>","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"64 11","pages":"5875–5884 5875–5884"},"PeriodicalIF":3.9000,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Manipulation of Oxygen Vacancy on a CeO2 Catalyst for the Carbonylation of Glycerol with CO2\",\"authors\":\"Bowen Tan, Danru Xu, Mengmeng Jin, Bolun Yang, Zhun Hu* and Jingjun Liu*, \",\"doi\":\"10.1021/acs.iecr.4c0439210.1021/acs.iecr.4c04392\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Cerium dioxide (CeO<sub>2</sub>) with different morphologies was synthesized via a hydrothermal method and applied to the carbonylation of glycerol with CO<sub>2</sub>. Subsequent characterization through H<sub>2</sub>-TPR and catalytic activity tests demonstrated that CeO<sub>2</sub> nanorods exhibited the highest oxygen storage/release capacity as well as enhanced catalytic performance compared to other morphologies. CeO<sub>2</sub> nanorods were thus further modified through hydrogen reduction at varying temperatures, aiming to tune the density of the oxygen vacancies. Characterization via BET, NH<sub>3</sub>-TPD, CO<sub>2</sub>-TPD, XPS, and ESR indicated that variations in morphology and reduction temperature influenced the microstructural characteristics and the strength of the acid–base sites of the catalysts. Notably, hydrogen reduction created more oxygen vacancies in the CeO<sub>2</sub> nanorods, with the concentration of these vacancies increasing with higher reduction temperatures. Furthermore, the catalytic activity of CeO<sub>2</sub> in glycerol carbonylation with CO<sub>2</sub> showed a positive correlation with the concentration of oxygen vacancies. Optimizing CeO<sub>2</sub> catalysts can enhance its performance in activating CO<sub>2</sub>, providing new ideas for industrial CO<sub>2</sub> resource utilization and carbon capture technology development.</p>\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"64 11\",\"pages\":\"5875–5884 5875–5884\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-03-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.iecr.4c04392\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.iecr.4c04392","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Manipulation of Oxygen Vacancy on a CeO2 Catalyst for the Carbonylation of Glycerol with CO2
Cerium dioxide (CeO2) with different morphologies was synthesized via a hydrothermal method and applied to the carbonylation of glycerol with CO2. Subsequent characterization through H2-TPR and catalytic activity tests demonstrated that CeO2 nanorods exhibited the highest oxygen storage/release capacity as well as enhanced catalytic performance compared to other morphologies. CeO2 nanorods were thus further modified through hydrogen reduction at varying temperatures, aiming to tune the density of the oxygen vacancies. Characterization via BET, NH3-TPD, CO2-TPD, XPS, and ESR indicated that variations in morphology and reduction temperature influenced the microstructural characteristics and the strength of the acid–base sites of the catalysts. Notably, hydrogen reduction created more oxygen vacancies in the CeO2 nanorods, with the concentration of these vacancies increasing with higher reduction temperatures. Furthermore, the catalytic activity of CeO2 in glycerol carbonylation with CO2 showed a positive correlation with the concentration of oxygen vacancies. Optimizing CeO2 catalysts can enhance its performance in activating CO2, providing new ideas for industrial CO2 resource utilization and carbon capture technology development.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.