{"title":"金/氧化锌催化剂上氧空位促进的乙二醇氧化酯化反应生成乙醇酸甲酯","authors":"Yanhong Quan, Zihui Qin, Xueyang Ren, Jun Ren","doi":"10.1016/j.apsusc.2024.161855","DOIUrl":null,"url":null,"abstract":"Au/ZnO-<em>x</em> with different morphologies were prepared by controlling the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> (<em>x</em>) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-<em>x</em> firstly increases and then decreases with the increase of the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub>, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (V<sub>o</sub><sup>+</sup>) accompanied with the highest <em>I</em><sub>100</sub>/<em>I</em><sub>101</sub> ratio at moderate (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> dosage, promoting the adsorption and dissociation of O<sub>2</sub> molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and irregular clusters, respectively. Significantly, it was found that there was a linear positive correlation between the V<sub>o</sub><sup>+</sup> and the EG conversion. Innovatively, the mechanism of the oxygen vacancy-catalyzed oxidative esterification of EG was proposed, which provided a new idea for the design of efficient catalysts for the reaction.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"13 1","pages":""},"PeriodicalIF":6.3000,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Oxygen vacancies-promoted oxidative esterification of ethylene glycol to methyl glycolate over Au/ZnO catalyst\",\"authors\":\"Yanhong Quan, Zihui Qin, Xueyang Ren, Jun Ren\",\"doi\":\"10.1016/j.apsusc.2024.161855\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Au/ZnO-<em>x</em> with different morphologies were prepared by controlling the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> (<em>x</em>) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-<em>x</em> firstly increases and then decreases with the increase of the amount of (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub>, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (V<sub>o</sub><sup>+</sup>) accompanied with the highest <em>I</em><sub>100</sub>/<em>I</em><sub>101</sub> ratio at moderate (NH<sub>4</sub>)<sub>2</sub>CO<sub>3</sub> dosage, promoting the adsorption and dissociation of O<sub>2</sub> molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and irregular clusters, respectively. Significantly, it was found that there was a linear positive correlation between the V<sub>o</sub><sup>+</sup> and the EG conversion. Innovatively, the mechanism of the oxygen vacancy-catalyzed oxidative esterification of EG was proposed, which provided a new idea for the design of efficient catalysts for the reaction.\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"13 1\",\"pages\":\"\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2024-11-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apsusc.2024.161855\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.apsusc.2024.161855","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Oxygen vacancies-promoted oxidative esterification of ethylene glycol to methyl glycolate over Au/ZnO catalyst
Au/ZnO-x with different morphologies were prepared by controlling the amount of (NH4)2CO3 (x) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-x firstly increases and then decreases with the increase of the amount of (NH4)2CO3, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (Vo+) accompanied with the highest I100/I101 ratio at moderate (NH4)2CO3 dosage, promoting the adsorption and dissociation of O2 molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and irregular clusters, respectively. Significantly, it was found that there was a linear positive correlation between the Vo+ and the EG conversion. Innovatively, the mechanism of the oxygen vacancy-catalyzed oxidative esterification of EG was proposed, which provided a new idea for the design of efficient catalysts for the reaction.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.