{"title":"La 改性 Cu/SiO2 在醋酸甲酯加氢反应中的催化性能","authors":"Chuanming ZHANG, Weijie LI, Jincan KANG, Lina LIN, Changxin LI, Lincai LI, Haoyu ZOU, Hongping ZHU","doi":"10.1016/S1872-5813(23)60382-2","DOIUrl":null,"url":null,"abstract":"<div><p>A series of Cu/SiO<sub>2</sub> catalysts modified with lanthanum (La) (30Cu-<em>n</em>La/SiO<sub>2</sub>, <em>n</em>=0, 0.5, 1 and 2) were synthesized using the ethanol (EtOH)-assisted ammonia-evaporation method; their catalytic performance in the gas-phase hydrogenation of methyl acetate (MeOAc) to produce ethanol (EtOH) was investigated. The results indicate that the catalytic performance of Cu/SiO<sub>2</sub> can be greatly enhanced by La modification. In particular, the 30Cu-0.5La/SiO<sub>2</sub> catalyst exhibits excellent performance in the MeOAc hydrogenation; under 230 °C, 2 MPa H<sub>2</sub>, an LHSV of 2 h<sup>-1</sup> and an H<sub>2</sub>/MeOAc molar ratio of 20, the MeOAc conversion reaches 98.5%, with a total EtOH yield of 97.0%. The N<sub>2</sub>-sorption, XRD, ICP-OES, H<sub>2</sub>-TPR, FT-IR, TEM, XPS, and AES characterization results reveal that the introduced La metal has a strong interaction with Cu, which can promote the dispersion of the copper species on the SiO<sub>2</sub> support. Moreover, the content of Cu<sup>+</sup> is increased significantly, which can enhance the electronic interaction with MeOAc via the acyl and methoxide groups and thus promote the hydrogenation of MeOAc to EtOH.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 131-139"},"PeriodicalIF":0.0000,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic performance of La-modified Cu/SiO2 in the hydrogenation of methyl acetate\",\"authors\":\"Chuanming ZHANG, Weijie LI, Jincan KANG, Lina LIN, Changxin LI, Lincai LI, Haoyu ZOU, Hongping ZHU\",\"doi\":\"10.1016/S1872-5813(23)60382-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A series of Cu/SiO<sub>2</sub> catalysts modified with lanthanum (La) (30Cu-<em>n</em>La/SiO<sub>2</sub>, <em>n</em>=0, 0.5, 1 and 2) were synthesized using the ethanol (EtOH)-assisted ammonia-evaporation method; their catalytic performance in the gas-phase hydrogenation of methyl acetate (MeOAc) to produce ethanol (EtOH) was investigated. The results indicate that the catalytic performance of Cu/SiO<sub>2</sub> can be greatly enhanced by La modification. In particular, the 30Cu-0.5La/SiO<sub>2</sub> catalyst exhibits excellent performance in the MeOAc hydrogenation; under 230 °C, 2 MPa H<sub>2</sub>, an LHSV of 2 h<sup>-1</sup> and an H<sub>2</sub>/MeOAc molar ratio of 20, the MeOAc conversion reaches 98.5%, with a total EtOH yield of 97.0%. The N<sub>2</sub>-sorption, XRD, ICP-OES, H<sub>2</sub>-TPR, FT-IR, TEM, XPS, and AES characterization results reveal that the introduced La metal has a strong interaction with Cu, which can promote the dispersion of the copper species on the SiO<sub>2</sub> support. Moreover, the content of Cu<sup>+</sup> is increased significantly, which can enhance the electronic interaction with MeOAc via the acyl and methoxide groups and thus promote the hydrogenation of MeOAc to EtOH.</p></div>\",\"PeriodicalId\":15956,\"journal\":{\"name\":\"燃料化学学报\",\"volume\":\"52 2\",\"pages\":\"Pages 131-139\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-02-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"燃料化学学报\",\"FirstCategoryId\":\"1087\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872581323603822\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"Energy\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"燃料化学学报","FirstCategoryId":"1087","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872581323603822","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Energy","Score":null,"Total":0}
Catalytic performance of La-modified Cu/SiO2 in the hydrogenation of methyl acetate
A series of Cu/SiO2 catalysts modified with lanthanum (La) (30Cu-nLa/SiO2, n=0, 0.5, 1 and 2) were synthesized using the ethanol (EtOH)-assisted ammonia-evaporation method; their catalytic performance in the gas-phase hydrogenation of methyl acetate (MeOAc) to produce ethanol (EtOH) was investigated. The results indicate that the catalytic performance of Cu/SiO2 can be greatly enhanced by La modification. In particular, the 30Cu-0.5La/SiO2 catalyst exhibits excellent performance in the MeOAc hydrogenation; under 230 °C, 2 MPa H2, an LHSV of 2 h-1 and an H2/MeOAc molar ratio of 20, the MeOAc conversion reaches 98.5%, with a total EtOH yield of 97.0%. The N2-sorption, XRD, ICP-OES, H2-TPR, FT-IR, TEM, XPS, and AES characterization results reveal that the introduced La metal has a strong interaction with Cu, which can promote the dispersion of the copper species on the SiO2 support. Moreover, the content of Cu+ is increased significantly, which can enhance the electronic interaction with MeOAc via the acyl and methoxide groups and thus promote the hydrogenation of MeOAc to EtOH.
期刊介绍:
Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.