Xiang-peng KONG , Xin-ming YOU , Pei-hong YUAN , Yue-huan WU , Rui-hong WANG , Jian-gang CHEN
{"title":"掺杂物对草酸二甲酯加氢制乙二醇Cu/ZnO催化剂结构及催化性能的影响","authors":"Xiang-peng KONG , Xin-ming YOU , Pei-hong YUAN , Yue-huan WU , Rui-hong WANG , Jian-gang CHEN","doi":"10.1016/S1872-5813(22)60073-2","DOIUrl":null,"url":null,"abstract":"<div><p>The Cu-<em>M</em>/ZnO catalysts (<em>M</em> = Zr<sup>4+</sup>, Al<sup>3+</sup> and Mg<sup>2+</sup>) for dimethyl oxalate (DMO) selective hydrogenation to ethylene glycol (EG) were synthesized by the co-precipitation method. The properties of the as-synthesized catalysts were characterized by N<sub>2</sub>-physisorption, N<sub>2</sub>O-titration, XRD, H<sub>2</sub>-TPR, CO<sub>2</sub>-TPD, SEM, FT-IR and XPS. It was found that the Cu dispersion could be effectively promoted by the dopants incorporated in the Cu/ZnO catalyst. Particularly, a trace amount of Mg<sup>2+</sup> and Al<sup>3+</sup> dopants could significantly reinforce the chemical interaction between the Cu and ZnO phases by embedding into the ZnO lattice, while the Cu/ZrO<sub>2</sub> interaction could be improved with the introduction of Zr<sup>4+</sup>. For DMO gas-phase hydrogenation, the EG yield of the Cu/ZnO catalyst increased from 75.0% to 85.0% and 90.0% in the presence of Zr<sup>4+</sup> and Al<sup>3+</sup> dopants, respectively. Particularly, the EG selectivity of Cu-Mg/ZnO catalyst reached up to 95.0% with DMO completely converted for more than 100 h. The correlation between the catalytic behavior and physicochemical features of the Cu/ZnO based catalysts suggested that the surface Cu<sup>+</sup> sites was vital for the catalytic behavior with adequate Cu<sup>0</sup> sites. Additionally, the strengthened Cu/oxide interaction favored the outstanding stability of the Cu-Zr/ZnO and Cu-Mg/ZnO catalyst for DMO hydrogenation.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Influence of dopants on the structure and catalytic features of the Cu/ZnO catalyst for dimethyl oxalate hydrogenation to ethylene glycol\",\"authors\":\"Xiang-peng KONG , Xin-ming YOU , Pei-hong YUAN , Yue-huan WU , Rui-hong WANG , Jian-gang CHEN\",\"doi\":\"10.1016/S1872-5813(22)60073-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The Cu-<em>M</em>/ZnO catalysts (<em>M</em> = Zr<sup>4+</sup>, Al<sup>3+</sup> and Mg<sup>2+</sup>) for dimethyl oxalate (DMO) selective hydrogenation to ethylene glycol (EG) were synthesized by the co-precipitation method. The properties of the as-synthesized catalysts were characterized by N<sub>2</sub>-physisorption, N<sub>2</sub>O-titration, XRD, H<sub>2</sub>-TPR, CO<sub>2</sub>-TPD, SEM, FT-IR and XPS. It was found that the Cu dispersion could be effectively promoted by the dopants incorporated in the Cu/ZnO catalyst. Particularly, a trace amount of Mg<sup>2+</sup> and Al<sup>3+</sup> dopants could significantly reinforce the chemical interaction between the Cu and ZnO phases by embedding into the ZnO lattice, while the Cu/ZrO<sub>2</sub> interaction could be improved with the introduction of Zr<sup>4+</sup>. For DMO gas-phase hydrogenation, the EG yield of the Cu/ZnO catalyst increased from 75.0% to 85.0% and 90.0% in the presence of Zr<sup>4+</sup> and Al<sup>3+</sup> dopants, respectively. Particularly, the EG selectivity of Cu-Mg/ZnO catalyst reached up to 95.0% with DMO completely converted for more than 100 h. The correlation between the catalytic behavior and physicochemical features of the Cu/ZnO based catalysts suggested that the surface Cu<sup>+</sup> sites was vital for the catalytic behavior with adequate Cu<sup>0</sup> sites. Additionally, the strengthened Cu/oxide interaction favored the outstanding stability of the Cu-Zr/ZnO and Cu-Mg/ZnO catalyst for DMO hydrogenation.</p></div>\",\"PeriodicalId\":15956,\"journal\":{\"name\":\"燃料化学学报\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2023-06-01\",\"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/S1872581322600732\",\"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/S1872581322600732","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"Energy","Score":null,"Total":0}
Influence of dopants on the structure and catalytic features of the Cu/ZnO catalyst for dimethyl oxalate hydrogenation to ethylene glycol
The Cu-M/ZnO catalysts (M = Zr4+, Al3+ and Mg2+) for dimethyl oxalate (DMO) selective hydrogenation to ethylene glycol (EG) were synthesized by the co-precipitation method. The properties of the as-synthesized catalysts were characterized by N2-physisorption, N2O-titration, XRD, H2-TPR, CO2-TPD, SEM, FT-IR and XPS. It was found that the Cu dispersion could be effectively promoted by the dopants incorporated in the Cu/ZnO catalyst. Particularly, a trace amount of Mg2+ and Al3+ dopants could significantly reinforce the chemical interaction between the Cu and ZnO phases by embedding into the ZnO lattice, while the Cu/ZrO2 interaction could be improved with the introduction of Zr4+. For DMO gas-phase hydrogenation, the EG yield of the Cu/ZnO catalyst increased from 75.0% to 85.0% and 90.0% in the presence of Zr4+ and Al3+ dopants, respectively. Particularly, the EG selectivity of Cu-Mg/ZnO catalyst reached up to 95.0% with DMO completely converted for more than 100 h. The correlation between the catalytic behavior and physicochemical features of the Cu/ZnO based catalysts suggested that the surface Cu+ sites was vital for the catalytic behavior with adequate Cu0 sites. Additionally, the strengthened Cu/oxide interaction favored the outstanding stability of the Cu-Zr/ZnO and Cu-Mg/ZnO catalyst for DMO hydrogenation.
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.