Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 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...

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Published in	Nature communications Vol. 10; no. 1; pp. 1166 - 10
Main Authors	Wang, Yuhao, Kattel, Shyam, Gao, Wengui, Li, Kongzhai, Liu, Ping, Chen, Jingguang G., Wang, Hua
Format	Journal Article
Language	English
Published	London Nature Publishing Group UK 11.03.2019 Nature Publishing Group Nature Portfolio
Subjects	639/638/77/885 639/638/77/887 639/638/898 Carbon dioxide Catalysis Catalysts catalytic mechanisms chemical engineering Copper Density functional theory Diffuse reflectance spectroscopy Fourier transforms heterogeneous catalysis Humanities and Social Sciences Hydrogen storage Hydrogenation INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Interfaces Methanol multidisciplinary Science Science (multidisciplinary) Zinc oxide Zirconium dioxide
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Abstract	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 . Despite great efforts, the reaction mechanism of CO 2 hydrogenation to methanol and the nature of the active sites on Cu–ZnO–ZrO 2 (CZZ) catalysts are still under debate. Herein, the authors report the interactions among the three components in controlling the catalytic performance of CZZ catalyst for CO 2 hydrogenation to methanol.
AbstractList	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. Despite great efforts, the reaction mechanism of CO2 hydrogenation to methanol and the nature of the active sites on Cu–ZnO–ZrO2 (CZZ) catalysts are still under debate. Herein, the authors report the interactions among the three components in controlling the catalytic performance of CZZ catalyst for CO2 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-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.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. 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 . Despite great efforts, the reaction mechanism of CO 2 hydrogenation to methanol and the nature of the active sites on Cu–ZnO–ZrO 2 (CZZ) catalysts are still under debate. Herein, the authors report the interactions among the three components in controlling the catalytic performance of CZZ catalyst for 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–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.Despite great efforts, the reaction mechanism of CO2 hydrogenation to methanol and the nature of the active sites on Cu–ZnO–ZrO2 (CZZ) catalysts are still under debate. Herein, the authors report the interactions among the three components in controlling the catalytic performance of CZZ catalyst for CO2 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 .
ArticleNumber	1166
Author	Wang, Yuhao Gao, Wengui Kattel, Shyam Li, Kongzhai Liu, Ping Chen, Jingguang G. Wang, Hua
Author_xml	– sequence: 1 givenname: Yuhao surname: Wang fullname: Wang, Yuhao organization: State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering, Kunming University of Science and Technology, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology – sequence: 2 givenname: Shyam surname: Kattel fullname: Kattel, Shyam organization: Chemistry Division, Brookhaven National Laboratory – sequence: 3 givenname: Wengui surname: Gao fullname: Gao, Wengui organization: State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering, Kunming University of Science and Technology, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology – sequence: 4 givenname: Kongzhai surname: Li fullname: Li, Kongzhai email: kongzhai.li@foxmail.com organization: State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering, Kunming University of Science and Technology, Department of Earth and Environmental Engineering, Columbia University – sequence: 5 givenname: Ping surname: Liu fullname: Liu, Ping organization: Chemistry Division, Brookhaven National Laboratory – sequence: 6 givenname: Jingguang G. surname: Chen fullname: Chen, Jingguang G. email: jgchen@columbia.edu organization: Chemistry Division, Brookhaven National Laboratory, Department of Chemical Engineering, Columbia University – sequence: 7 givenname: Hua surname: Wang fullname: Wang, Hua email: wanghua65@163.com organization: State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering, Kunming University of Science and Technology, School of Pharmacy and Chemistry, Dali University
BackLink	https://www.osti.gov/servlets/purl/1504379$$D View this record in Osti.gov
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Snippet	The synergistic interaction among different components in complex catalysts is one of the crucial factors in determining catalytic performance. Here we report... Despite great efforts, the reaction mechanism of CO2 hydrogenation to methanol and the nature of the active sites on Cu–ZnO–ZrO2 (CZZ) catalysts are still...
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SubjectTerms	639/638/77/885 639/638/77/887 639/638/898 Carbon dioxide Catalysis Catalysts catalytic mechanisms chemical engineering Copper Density functional theory Diffuse reflectance spectroscopy Fourier transforms heterogeneous catalysis Humanities and Social Sciences Hydrogen storage Hydrogenation INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Interfaces Methanol multidisciplinary Science Science (multidisciplinary) Zinc oxide Zirconium dioxide
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Title	Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 hydrogenation to methanol
URI	https://link.springer.com/article/10.1038/s41467-019-09072-6 https://www.proquest.com/docview/2190075914 https://www.proquest.com/docview/2190491534 https://www.osti.gov/servlets/purl/1504379 https://pubmed.ncbi.nlm.nih.gov/PMC6411953 https://doaj.org/article/f8d2747cf4c14ab7b7fb442bdd882ab7
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