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Nano Research 2023, 16(4): 4582-4588 https://doi.org/10.1007/s12274-022-4862-9
Research Article | Issue | Published: 16 September 2022

Cu1-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO2 electroreduction

Show Author's Information Konglin Wu1,2,3,  Zhaobin Fang1,3,  Cheng Peng1,3,  Yining Zhang4,5,  Binbin Jiang6,  Yanshang Kang1,3,  Zhiming Chen2,  Mingfu Ye1,3,7,  Yuxi Wu1,  Xianwen Wei1,3,  Shoujie Liu4( ),  Sha Li4( ),  Jian Zhang8( )
Key Laboratory of Metallurgical Emission Reduction & Resources Recycling of Ministry of Education, Anhui University of Technology, Maanshan 243002, China
Anhui Laboratory of Clean Catalytic Engineering, School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu 241000, China
Institute of Clean Energy and Advanced Nanocatalysis (iClean), School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, China
Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515063, China
Institute of Molecular Plus, Tianjin University, Tianjin 300072, China
School of Chemistry and Chemical Engineering, Anqing Normal University, Anqing 246001, China
Jiangxi Province Engineering Research Center of Ecological Chemical Industry, Jiujiang University, Jiujiang 332005, China
College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, China
Keywords:
porous carbon, single-atom catalysis, dual-active sites, dehydrogenative coupling
Topics:
Catalysts
Cite this article:
Wu K, Fang Z, Peng C, et al. Cu1-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO2 electroreduction. Nano Research, 2023, 16(4): 4582-4588. https://doi.org/10.1007/s12274-022-4862-9
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Abstract Full text Electronic supplementary material About this article

Dual-active sites (DASs) catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects. Therefore, the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now. In this work, we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material (Cu1-B/NPC). Numerous systematic characterization and density functional theoretical (DFT) calculation results showed that the Cu and B existed as Cu-N4 porphyrin-like unit and B-N3 unit in the obtained catalyst. DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu1-B-N6 dual-sites. The Cu1-B/NPC catalyst was more effective than the single-active site catalysts with B-N3 sites in NPC (B/NPC) and Cu-N4 porphyrin-like sites in NPC (Cu1/NPC), respectively, for the dehydrogenative coupling of dimethylphenylsilane (DiMPSH) with various alcohols, performing the great activity (> 99%) and selectivity (> 99%). The catalytic performances of the Cu1-B/NPC catalyst remained nearly unchanged after five cycles, also indicating its outstanding recyclability. DFT calculations showed that the Cu1-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N3 and Cu-N4 porphyrin-like sites. Furthermore, the rate-limiting step of dehydrogenation of DiMPSH on Cu1-B-N6 dual-sites also showed a much lower activation energy than the other two single sites. Benefitting from the superiority of the Cu1-B-N6 dual-sites, the Cu1-B/NPC catalyst can also be used for CO2 electroreduction to produce syngas. Thus, DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.


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Abstract
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Electronic supplementary material
About this article

Cu1-B dual-active sites catalysts for the efficient dehydrogenative coupling and CO2 electroreduction

Show Author's information Konglin Wu1,2,3, Zhaobin Fang1,3, Cheng Peng1,3, Yining Zhang4,5, Binbin Jiang6, Yanshang Kang1,3, Zhiming Chen2, Mingfu Ye1,3,7, Yuxi Wu1, Xianwen Wei1,3, Shoujie Liu4( ), Sha Li4( ), Jian Zhang8( )
Key Laboratory of Metallurgical Emission Reduction & Resources Recycling of Ministry of Education, Anhui University of Technology, Maanshan 243002, China
Anhui Laboratory of Clean Catalytic Engineering, School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu 241000, China
Institute of Clean Energy and Advanced Nanocatalysis (iClean), School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, China
Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515063, China
Institute of Molecular Plus, Tianjin University, Tianjin 300072, China
School of Chemistry and Chemical Engineering, Anqing Normal University, Anqing 246001, China
Jiangxi Province Engineering Research Center of Ecological Chemical Industry, Jiujiang University, Jiujiang 332005, China
College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, China

Abstract

Dual-active sites (DASs) catalysts have positive potential applications in broad fields because of their specific active sites and synergistic catalytic effects. Therefore, the controllable synthesis and finely regulating the activity of such catalysts has become a hot research area for now. In this work, we developed a pyrolysis-etching-hydrogen activation strategy to prepare the DASs catalysts involving single-atom Cu and B on N-doped porous carbon material (Cu1-B/NPC). Numerous systematic characterization and density functional theoretical (DFT) calculation results showed that the Cu and B existed as Cu-N4 porphyrin-like unit and B-N3 unit in the obtained catalyst. DFT calculations further revealed that single-atom Cu and B sites were linked by bridging N atoms to form the Cu1-B-N6 dual-sites. The Cu1-B/NPC catalyst was more effective than the single-active site catalysts with B-N3 sites in NPC (B/NPC) and Cu-N4 porphyrin-like sites in NPC (Cu1/NPC), respectively, for the dehydrogenative coupling of dimethylphenylsilane (DiMPSH) with various alcohols, performing the great activity (> 99%) and selectivity (> 99%). The catalytic performances of the Cu1-B/NPC catalyst remained nearly unchanged after five cycles, also indicating its outstanding recyclability. DFT calculations showed that the Cu1-B-N6 dual-sites exhibited the lowest energy profile on the potential energy surface than that of sole B-N3 and Cu-N4 porphyrin-like sites. Furthermore, the rate-limiting step of dehydrogenation of DiMPSH on Cu1-B-N6 dual-sites also showed a much lower activation energy than the other two single sites. Benefitting from the superiority of the Cu1-B-N6 dual-sites, the Cu1-B/NPC catalyst can also be used for CO2 electroreduction to produce syngas. Thus, DASs catalysts are promising to achieve multifunctional catalytic properties and have aroused positive attention in the field of catalysis.

Keywords: porous carbon, single-atom catalysis, dual-active sites, dehydrogenative coupling

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Publication history
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Acknowledgements

Publication history

Received: 06 July 2022
Revised: 02 August 2022
Accepted: 03 August 2022
Published: 16 September 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51902003, 22002085, 21771003, 21501004), the University Synergy Innovation Program of Anhui Province (No. GXXT-2021-020), the Anhui Province Natural Science Foundation (Nos. 2108085QB71 and 2008085QB53), the Natural Science Research Project of Anhui Province Education Department (No. KJ2019A0581), the Open Project of Key Laboratory of Metallurgical Emission Reduction & Resources Recycling of Ministry of Education (No. JKF21-03), the Open Foundation of Anhui Laboratory of Clean Catalytic Engineering (No. LCCE-01), and the Open Research Funds of Jiangxi Province Engineering Research Center of Ecological Chemical Industry (STKF2109). We acknowledge the 1W1B beamline station of Beijing Synchrotron Radiation Facility (BSRF), the Institute of Physics of Chinese Academy of Sciences, and the National Synchrotron Radiation Laboratory (NSRL) of Hefei. We also thank Prof. L. R. Zheng, Prof. W. S. Yan, and Prof. Q. H. Zhang for their help in catalyst characterizations. Thanks to Prof. C. Chen and Dr. W. -C. Cheong of Tsinghua University for their help in materials characterizations.

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