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Capsule-Structured Copper-Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol
Guo, Yongle; Guo, Xinwen; Song, Chunshan; Han, Xinghua; Liu, Hongyang; Zhao, Zhongkui
2019-11-22
Source PublicationCHEMSUSCHEM
ISSN1864-5631
Volume12Issue:22Pages:4916-4926
AbstractTo 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.
Keywordcarbon dioxide hydrogenation core-shell structure heterogeneous catalysis methanol synthesis
Indexed BySCI
Language英语
WOS IDWOS:000494249800001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Cited Times:1[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/80689
Collection中国科学院金属研究所
Recommended Citation
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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