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Capsule-Structured Copper-Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol

文献类型：期刊论文

作者Guo, Yongle2; Guo, Xinwen2; Song, Chunshan2,3,4,5; Han, Xinghua1; Liu, Hongyang6; Zhao, Zhongkui2
刊名CHEMSUSCHEM
出版日期2019-11-22
卷号12期号:22页码:4916-4926
关键词carbon dioxide hydrogenation core-shell structure heterogeneous catalysis methanol synthesis
ISSN号1864-5631
DOI10.1002/cssc.201902485
通讯作者Han, Xinghua(hxh@nuc.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Zhao, Zhongkui(zkzhao@dlut.edu.cn)
英文摘要To develop a new and efficient CO2-to-methanol catalyst is of extreme significance but still remains a challenge. Herein, an innovative indirect two-step strategy is reported to synthesize a highly efficient capsule-structured copper-based CO2-to-methanol catalyst (CZA-r@CZM). It consists of a structurally reconstructed millimeter-sized Cu/ZnO/Al2O3 core (CZA-r) with intensified Cu-ZnO interactions, which is made by a facile hydrothermal treatment in an alkaline aqueous solution, and a Cu/ZnO/MgO (CZM) shell prepared by an ethylene glycol-assisted physical coating method. The CZA-r core displays 2.7 times higher CO2 hydrogenation activity with 2.0 times higher CO selectivity than the previously reported Cu/ZnO/Al2O3 (CZA-p), whereas the CZM shell can efficiently catalyze hydrogenation of the as-formed CO from the CZA-r core to methanol as it passes through the shell. As a result, the developed capsule-structured CZA-r@CZM catalyst exhibits 2.4 times higher CO2 conversion with 1.8 times higher turnover frequency and 2.3-fold higher methanol space-time yield than the CZA-p catalyst (729.8 vs. 312.6 g(MeOH) kg(cat)(-1) h(-1)). In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) experiments reveal that the CO2 hydrogenation reaction proceeds through a reverse water-gas shift reaction followed by a CO hydrogenation pathway via an *H3CO intermediate. This work not only produces an efficient CO2-to-methanol catalyst, but also opens a new avenue for designing superior catalysts for other consecutive transformations.
资助项目National Natural Science Foundation of China[U1610104] ; Chinese Ministry of Education via the Program for New Century Excellent Talents in Universities[NCET-12-0079]
WOS研究方向Chemistry ; Science & Technology - Other Topics
语种英语
WOS记录号WOS:000494249800001
出版者WILEY-V C H VERLAG GMBH
资助机构National Natural Science Foundation of China ; Chinese Ministry of Education via the Program for New Century Excellent Talents in Universities
源URL[http://ir.imr.ac.cn/handle/321006/136956]  
专题金属研究所_中国科学院金属研究所
通讯作者Han, Xinghua; Liu, Hongyang; Zhao, Zhongkui
作者单位1.North Univ China, Sch Chem Engn & Technol, Taiyuan 030051, Shanxi, Peoples R China
2.Dalian Univ Technol, PSU DUT Joint Ctr Energy Res, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China
3.Penn State Univ, PSU DUT Joint Ctr Energy Res, EMS Energy Inst, University Pk, PA 16802 USA
4.Penn State Univ, Dept Energy & Mineral Engn, University Pk, PA 16802 USA
5.Penn State Univ, Dept Chem Engn, University Pk, PA 16802 USA
6.Chinese Acad Sci, Shenyang Res Ctr Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式
GB/T 7714		 Guo, Yongle,Guo, Xinwen,Song, Chunshan,et al. Capsule-Structured Copper-Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol[J]. CHEMSUSCHEM,2019,12(22):4916-4926.
APA Guo, Yongle,Guo, Xinwen,Song, Chunshan,Han, Xinghua,Liu, Hongyang,&Zhao, Zhongkui.(2019).Capsule-Structured Copper-Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol.CHEMSUSCHEM,12(22),4916-4926.
MLA Guo, Yongle,et al."Capsule-Structured Copper-Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol".CHEMSUSCHEM 12.22(2019):4916-4926.

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来源：金属研究所

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