Hydrogenation of gamma-Butyrolactone to 1,4-Butanediol over CuCo/TiO2 Bimetallic Catalysts | |
Xu, Zhuoran1; George W. Huber1; James A. Dumesic1; Zachary J. Brentzel1; Joseph P. Chada1; Kevin J. Barnett1; Huang ZW(黄志威)1,2![]() | |
刊名 | ACS Catalysis
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2017 | |
卷号 | 7期号:12页码:8429-8440 |
关键词 | Cuco Bimetallic Catalyst Hydrogenation Gamma-butyrolactone Reaction Pathway And Mechanism 1 4-butanediol |
ISSN号 | 2155-5435 |
DOI | 10.1021/acscatal.7b03016 |
英文摘要 | Titania-supported monometallic and bimetallic Cu–Co catalysts were prepared using (co)impregnation and studied for the hydrogenation of γ-butyrolactone (GBL) to 1,4-butanediol (BDO) at temperatures from 100 to 180 °C and a hydrogen pressure of 3.4 MPa. The highest catalytic activity occurred at a Cu:Co atomic ratio of 1:9 (Cu0.1Co0.9/TiO2), and a 95% yield of BDO was obtained. Characterization results showed mainly small nanoparticles (average size 2.6 nm) for pure Cu/TiO2, large particles (∼19.8 nm) for pure Co/TiO2, and a bimodal particle size distribution of both small (∼2.3 nm) and large (∼16.5 nm) particles for the bimetallic catalyst with a Cu:Co ratio of 1:1. The addition of ∼10 mol % Cu to Co/TiO2 increased the reducibility of the Co and resulted in the formation of core–shell CuCo bimetallic nanoparticles with a Co-rich core and Cu-rich shell. GBL hydrogenation in liquid ethanol and water produced an ester (ethyl 4-hydroxybutanoate) and a carboxylic acid (4-hydroxybutanoic acid) as the major products, respectively. GBL hydrogenation in 1,4-dioxane likely went through a 2-hydroxytetrahydrofuran (2-HTHF) intermediate. The 2-HTHF underwent facile ring-opening tautomerization to 4-hydroxybutanal (4-HB), followed by rapid hydrogenation to BDO at a reaction rate up to 700 times faster than GBL hydrogenation. The Cu0.1Co0.9/TiO2 catalyst maintained the BDO selectivity and about 80% of initial activity for GBL hydrogenation after 150 h time on stream in a continuous flow reactor. |
学科主题 | 物理化学与绿色催化 |
资助项目 | 分子催化与技术研究组 |
语种 | 英语 |
WOS记录号 | WOS:000417230500049 |
资助机构 | the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), under Award Number DE-EE0006878;the National Science Foundation Engineering Research Center for Biorenewable Chemicals (CBiRC), under Award No. EEC-0813570;The facilities and instrumentation for microscopy at UW-Madison were supported by the University of Wisconsin Materials Research Science and Engineering Center (DMR-1121288); the China Scholarship Council for the Visiting Scholars Program (File No. 201604910003);the National Natural Science Foundation of China (Grant No. 21473224);the Youth Innovation Promotion Association, CAS |
内容类型 | 期刊论文 |
源URL | [http://ir.licp.ac.cn/handle/362003/23797] ![]() |
专题 | 兰州化学物理研究所_OSSO国家重点实验室 |
通讯作者 | George W. Huber |
作者单位 | 1.Univ Wisconsin Madison, Dept Chem & Biol Engn, Madison, WI 53706 USA 2.Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Lanzhou Inst Chem Phys, Lanzhou 730000, Gansu, Peoples R China |
推荐引用方式 GB/T 7714 | Xu, Zhuoran,George W. Huber,James A. Dumesic,et al. Hydrogenation of gamma-Butyrolactone to 1,4-Butanediol over CuCo/TiO2 Bimetallic Catalysts[J]. ACS Catalysis,2017,7(12):8429-8440. |
APA | Xu, Zhuoran.,George W. Huber.,James A. Dumesic.,Zachary J. Brentzel.,Joseph P. Chada.,...&Huang ZW.(2017).Hydrogenation of gamma-Butyrolactone to 1,4-Butanediol over CuCo/TiO2 Bimetallic Catalysts.ACS Catalysis,7(12),8429-8440. |
MLA | Xu, Zhuoran,et al."Hydrogenation of gamma-Butyrolactone to 1,4-Butanediol over CuCo/TiO2 Bimetallic Catalysts".ACS Catalysis 7.12(2017):8429-8440. |
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