Synergetic Catalysis of Bimetallic CuCo Nanocomposites for Selective Hydrogenation of Bioderived Esters | |
Department | OSSO国家重点实验室 |
Wu J(吴君)1,2; Gao G(高广)1; Sun P(孙鹏)1; Long XD(龙向东)1,2; Li FW(李福伟)1; Li FW(李福伟) | |
2017 | |
Source Publication | ACS Catalysis |
ISSN | 2155-5435 |
Volume | 7Issue:11Pages:7890-7901 |
Abstract | Bimetallic catalysts based on nonprecious transition metals have attracted increasing attention because of their unique synergistic effects in catalytic reactions, but the understanding of the nature of synergistic effects and their roles in a specific hydrogenation reaction remains lacking. Herein, a series of bimetallic CuxCoy/Al2O3 (x/y = 5:1, 2:1, 1:1, 1:2, 1:5) nanocomposite catalysts were fabricated via the successive calcination and reductive activation process of layered double hydroxide precursors. Their catalytic performance in the selective hydrogenation of bioderived ethyl levulinate to 1,4-pentanediol (1,4-PeD) depended sensitively on the chemical composition of bimetallic CuCo catalysts. The optimal bimetallic Cu2Co1/Al2O3 catalyst exhibited markedly improved catalytic activity and selectivity compared to monometallic Cu/Al2O3, as confirmed by its lower apparent activation energy barrier of 65.1 kJ mol–1 of the rate-determining step and its high selectivity of 93% to 1,4-PeD. Detailed characterization analyses and intrinsic catalytic studies revealed that the presence of CoOx species in the bimetallic CuxCoy/Al2O3 catalysts enhanced the metallic Cu dispersion and H2 activation ability. More importantly, the strong electronic interaction at the interface of Cu and adjacent CoOx species modified the chemical states of Cu species to create proper surface Cu0/Cu+ distributions and, particularly, provided synergic catalysis sites of Cu and electron-deficient CoOx species, which was primarily responsible for the excellent catalytic performance of bimetallic CuCo catalysts. The bimetallic CuCo catalysts exhibited good stability in both batch and fixed-bed continuous flow reactions. Furthermore, present CuCo nanocomposite catalyst could be applied to the highly selective hydrogenation of other carboxylic esters and lactones to synthesize valuable C4, C5, and C6 diols. |
Keyword | Synergetic Catalysis Cuco Nanocomposite Layered Double Hydroxide Selective Hydrogenation Diol Monomer |
Subject Area | 物理化学与绿色催化 |
DOI | 10.1021/acscatal.7b02837 |
Funding Organization | the National Natural Science Foundation of China (21773271;21503242;21522309;21373246);the Chinese Academy of Sciences |
Indexed By | SCI |
If | 10.614 |
Language | 英语 |
Funding Project | 均相催化课题组 |
compositor | 第一作者单位 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/22682 |
Collection | 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Li FW(李福伟) |
Affiliation | 1.State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, P. R. China 2.University of Chinese Academy of Sciences, Beijing 100039, P. R. China |
Recommended Citation GB/T 7714 | Wu J,Gao G,Sun P,et al. Synergetic Catalysis of Bimetallic CuCo Nanocomposites for Selective Hydrogenation of Bioderived Esters[J]. ACS Catalysis,2017,7(11):7890-7901. |
APA | Wu J,Gao G,Sun P,Long XD,Li FW,&李福伟.(2017).Synergetic Catalysis of Bimetallic CuCo Nanocomposites for Selective Hydrogenation of Bioderived Esters.ACS Catalysis,7(11),7890-7901. |
MLA | Wu J,et al."Synergetic Catalysis of Bimetallic CuCo Nanocomposites for Selective Hydrogenation of Bioderived Esters".ACS Catalysis 7.11(2017):7890-7901. |
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