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Title: Exploring the ternary interactions in Cu–ZnO–ZrO 2 catalysts for efficient CO 2 hydrogenation to methanol

The synergistic interaction among different components in complex catalysts is one of the crucial factors in determining catalytic performance. Here we report the interactions among the three components in controlling the catalytic performance of Cu–ZnO–ZrO 2 (CZZ) catalyst for CO 2 hydrogenation to methanol. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements under the activity test pressure (3 MPa) reveal that the CO 2 hydrogenation to methanol on the CZZ catalysts follows the formate pathway. Density functional theory (DFT) calculations agree with the in situ DRIFTS measurements, showing that the ZnO–ZrO 2 interfaces are the active sites for CO 2 adsorption and conversion, while the presence of metallic Cu is also necessary to facilitate H 2 dissociation and to provide hydrogen resource. The combined experiment and DFT results reveal that tuning the interaction between ZnO and ZrO 2 can be considered as another important factor for designing high performance catalysts for methanol generation from CO 2.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [2] ;  [4] ;  [5]
  1. Kunming Univ. of Science and Technology (China). State Key Lab. of Complex Nonferrous Metal Resources Clean Utilization Engineering. Faculty of Metallurgical and Energy Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  3. Kunming Univ. of Science and Technology (China). State Key Lab. of Complex Nonferrous Metal Resources Clean Utilization Engineering; Columbia Univ., New York, NY (United States). Dept. of Earth and Environmental Engineering
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
  5. Kunming Univ. of Science and Technology (China). State Key Lab. of Complex Nonferrous Metal Resources Clean Utilization Engineering; Dali Univ. (China). School of Pharmacy and Chemistry
Publication Date:
Report Number(s):
BNL-211494-2019-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:
SC0012704; AC02-05CH11231; 51774159; 51304099; 51404122; 2011BAC01B03; 2014HB006
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States); Kunming Univ. of Science and Technology (China)
Sponsoring Org:
USDOE Office of Science (SC); National Natural Science Foundation of China (NNSFC); National Key Technologies R & D Program of China; Candidate Talents Training Fund of Yunnan Province (China)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalytic mechanisms; chemical engineering; heterogeneous catalysis
OSTI Identifier:
1504379

Wang, Yuhao, Kattel, Shyam, Gao, Wengui, Li, Kongzhai, Liu, Ping, Chen, Jingguang G., and Wang, Hua. Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 hydrogenation to methanol. United States: N. p., Web. doi:10.1038/s41467-019-09072-6.
Wang, Yuhao, Kattel, Shyam, Gao, Wengui, Li, Kongzhai, Liu, Ping, Chen, Jingguang G., & Wang, Hua. Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 hydrogenation to methanol. United States. doi:10.1038/s41467-019-09072-6.
Wang, Yuhao, Kattel, Shyam, Gao, Wengui, Li, Kongzhai, Liu, Ping, Chen, Jingguang G., and Wang, Hua. 2019. "Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 hydrogenation to methanol". United States. doi:10.1038/s41467-019-09072-6. https://www.osti.gov/servlets/purl/1504379.
@article{osti_1504379,
title = {Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 hydrogenation to methanol},
author = {Wang, Yuhao and Kattel, Shyam and Gao, Wengui and Li, Kongzhai and Liu, Ping and Chen, Jingguang G. and Wang, Hua},
abstractNote = {The synergistic interaction among different components in complex catalysts is one of the crucial factors in determining catalytic performance. Here we report the interactions among the three components in controlling the catalytic performance of Cu–ZnO–ZrO2 (CZZ) catalyst for CO2 hydrogenation to methanol. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements under the activity test pressure (3 MPa) reveal that the CO2 hydrogenation to methanol on the CZZ catalysts follows the formate pathway. Density functional theory (DFT) calculations agree with the in situ DRIFTS measurements, showing that the ZnO–ZrO2 interfaces are the active sites for CO2 adsorption and conversion, while the presence of metallic Cu is also necessary to facilitate H2 dissociation and to provide hydrogen resource. The combined experiment and DFT results reveal that tuning the interaction between ZnO and ZrO2 can be considered as another important factor for designing high performance catalysts for methanol generation from CO2.},
doi = {10.1038/s41467-019-09072-6},
journal = {Nature Communications},
number = ,
volume = 10,
place = {United States},
year = {2019},
month = {3}
}

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