Title: Hybrid Catalyst Coupling Zn Single Atoms and CuN<sub>x</sub> Clusters for Synergetic Catalytic Reduction of CO<sub>2</sub>
Abstract: Advanced Functional MaterialsVolume 33, Issue 16 2214215 Research Article Hybrid Catalyst Coupling Zn Single Atoms and CuNx Clusters for Synergetic Catalytic Reduction of CO2 Xiaosong Hu, Xiaosong Hu College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. China Key Laboratory of 3D Micro/Nano Fabrication and Characterization of Zhejiang Province, School of Engineering, Westlake University, Hangzhou, Zhejiang Province, 310024 P. R. ChinaSearch for more papers by this authorXinyu Liu, Xinyu Liu College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. ChinaSearch for more papers by this authorXin Hu, Xin Hu College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. ChinaSearch for more papers by this authorChaoyue Zhao, Chaoyue Zhao College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. ChinaSearch for more papers by this authorQingxin Guan, Corresponding Author Qingxin Guan [email protected] College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. China E-mail: [email protected]; [email protected]Search for more papers by this authorWei Li, Corresponding Author Wei Li [email protected] orcid.org/0000-0001-7287-8523 College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. China E-mail: [email protected]; [email protected]Search for more papers by this author Xiaosong Hu, Xiaosong Hu College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. China Key Laboratory of 3D Micro/Nano Fabrication and Characterization of Zhejiang Province, School of Engineering, Westlake University, Hangzhou, Zhejiang Province, 310024 P. R. ChinaSearch for more papers by this authorXinyu Liu, Xinyu Liu College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. ChinaSearch for more papers by this authorXin Hu, Xin Hu College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. ChinaSearch for more papers by this authorChaoyue Zhao, Chaoyue Zhao College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. ChinaSearch for more papers by this authorQingxin Guan, Corresponding Author Qingxin Guan [email protected] College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. China E-mail: [email protected]; [email protected]Search for more papers by this authorWei Li, Corresponding Author Wei Li [email protected] orcid.org/0000-0001-7287-8523 College of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin, 300071 P. R. China E-mail: [email protected]; [email protected]Search for more papers by this author First published: 02 February 2023 https://doi.org/10.1002/adfm.202214215Citations: 1Read the full textAboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onEmailFacebookTwitterLinkedInRedditWechat Abstract Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO2 hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnNx@C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N4 sites and low valence CuNx clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N4 and N4 structures, which show strong Lewis basicity and has strong adsorption for *CO2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO2. In the catalytic process, CuNx not only adsorbs and activates H2, but also cooperates with the adjacent Zn-N4 and N4 structures to jointly activate CO2 molecules and further promotes the hydrogenation of CO2. This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts. Conflict of Interest The authors declare no conflict of interest. Open Research Data Availability Statement The data that support the findings of this study are available from the corresponding author upon reasonable request. Supporting Information Filename Description adfm202214215-sup-0001-SuppMat.pdf3.4 MB Supporting Information Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article. References 1a) G. Wang, J. Chen, Y. Ding, P. Cai, L. Yi, Y. Li, C. Tu, Y. Hou, Z. Wen, L. Dai, Chem. Soc. Rev. 2021, 50, 4993; 10.1039/D0CS00071J CASPubMedWeb of Science®Google Scholarb) A. P. Soleymani, L. R. Parent, J. Jankovic, Adv. Funct. 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Publication Year: 2023
Publication Date: 2023-02-02
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