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

doi:10.1002/cssc.201902485

IMR OpenIR

	Capsule-Structured Copper-Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol
	Guo, Yongle 1; Guo, Xinwen 1; Song, Chunshan 1,2,3,4; Han, Xinghua 5; Liu, Hongyang 6; Zhao, Zhongkui 1
通讯作者	Han, Xinghua(hxh@nuc.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) ; Zhao, Zhongkui(zkzhao@dlut.edu.cn)
	2019-11-22
发表期刊	CHEMSUSCHEM
ISSN	1864-5631
卷号	12 期号:22 页码:4916-4926
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.
关键词	carbon dioxide hydrogenation core-shell structure heterogeneous catalysis methanol synthesis
资助者	National Natural Science Foundation of China ; Chinese Ministry of Education via the Program for New Century Excellent Talents in Universities
DOI	10.1002/cssc.201902485
收录类别	SCI
语种	英语
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
WOS类目	Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology
WOS记录号	WOS:000494249800001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：20[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/136957
专题	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.Dalian Univ Technol, PSU DUT Joint Ctr Energy Res, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China 2.Penn State Univ, PSU DUT Joint Ctr Energy Res, EMS Energy Inst, University Pk, PA 16802 USA 3.Penn State Univ, Dept Energy & Mineral Engn, University Pk, PA 16802 USA 4.Penn State Univ, Dept Chem Engn, University Pk, PA 16802 USA 5.North Univ China, Sch Chem Engn & Technol, Taiyuan 030051, Shanxi, Peoples R China 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.