{"title":"基于密度泛函理论的Ni4/MCM-41催化剂合成气甲烷化机理研究","authors":"Jiaying Zhang","doi":"10.1177/1468678319854871","DOIUrl":null,"url":null,"abstract":"The density functional theory method is employed to systematically explore the mechanism of syngas methanation on the Ni4/MCM-41 catalyst surface. The calculation results show that the optimal pathway of CH4 formation is CO + H → CHO + H → CH2O + H → CH3O → CH3 + H → CH4 with the rate-determining step of CH3O direct dissociation. Because the activation energy for the direct dissociation of CH3O species is much lower than that for the CH3OH formation (198.6 vs 264.8 kJ mol−1), there is almost no by-product CH3OH that appeared in the products of the syngas methanation over the Ni4/MCM-41 catalyst. Compared with other conventional nickel-based methanation catalysts, Ni4/MCM-41 catalyst is an excellent methanation catalyst with high selectivity of CH4.","PeriodicalId":20859,"journal":{"name":"Progress in Reaction Kinetics and Mechanism","volume":"54 1","pages":"222 - 233"},"PeriodicalIF":2.1000,"publicationDate":"2019-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"1","resultStr":"{\"title\":\"Study on syngas methanation mechanism over Ni4/MCM-41 catalyst based on density functional theory\",\"authors\":\"Jiaying Zhang\",\"doi\":\"10.1177/1468678319854871\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The density functional theory method is employed to systematically explore the mechanism of syngas methanation on the Ni4/MCM-41 catalyst surface. The calculation results show that the optimal pathway of CH4 formation is CO + H → CHO + H → CH2O + H → CH3O → CH3 + H → CH4 with the rate-determining step of CH3O direct dissociation. Because the activation energy for the direct dissociation of CH3O species is much lower than that for the CH3OH formation (198.6 vs 264.8 kJ mol−1), there is almost no by-product CH3OH that appeared in the products of the syngas methanation over the Ni4/MCM-41 catalyst. Compared with other conventional nickel-based methanation catalysts, Ni4/MCM-41 catalyst is an excellent methanation catalyst with high selectivity of CH4.\",\"PeriodicalId\":20859,\"journal\":{\"name\":\"Progress in Reaction Kinetics and Mechanism\",\"volume\":\"54 1\",\"pages\":\"222 - 233\"},\"PeriodicalIF\":2.1000,\"publicationDate\":\"2019-06-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"1\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Progress in Reaction Kinetics and Mechanism\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1177/1468678319854871\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Progress in Reaction Kinetics and Mechanism","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1177/1468678319854871","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Study on syngas methanation mechanism over Ni4/MCM-41 catalyst based on density functional theory
The density functional theory method is employed to systematically explore the mechanism of syngas methanation on the Ni4/MCM-41 catalyst surface. The calculation results show that the optimal pathway of CH4 formation is CO + H → CHO + H → CH2O + H → CH3O → CH3 + H → CH4 with the rate-determining step of CH3O direct dissociation. Because the activation energy for the direct dissociation of CH3O species is much lower than that for the CH3OH formation (198.6 vs 264.8 kJ mol−1), there is almost no by-product CH3OH that appeared in the products of the syngas methanation over the Ni4/MCM-41 catalyst. Compared with other conventional nickel-based methanation catalysts, Ni4/MCM-41 catalyst is an excellent methanation catalyst with high selectivity of CH4.