Doping sp-hybridized B atoms in graphyne supported single cobalt atoms for hydrogen evolution electrocatalysis |
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| Affiliation: | 1. School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China;2. School of Chemical Engineering, Sichuan University, Chengdu 610065, China;3. Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China;1. School of Electric Power, North China University of Water Resources and Electric Power, Zhengzhou 450045, China;2. Key Laboratory of Low-grade Energy Utilization Technologies and Systems (Chongqing University), Ministry of Education, Chongqing 400044, China;3. School of Environmental and Municipal Engineering, North China University of Water Resources and Electric Power, Zhengzhou 450045, China;1. University of Genova, Dipartimento di Farmacia, Viale Cembrano 4, 16148 Genova, Italy;2. INSTM, UdR Genova, Via Dodecaneso 31, 16146 Genova, Italy;3. University of Genova, Dipartimento di Ingegneria Civile, Chimica e Ambientale, Via all’Opera Pia 15, 16145, Italy;4. University of Genova, Dipartimento di Chimica e Chimica Industriale, Via Dodecaneso, 31, 16146 Genova, Italy;1. Graduate School of Natural and Applied Sciences, Gazi University, 06500, Teknikokullar, Ankara, Turkey;2. Department of Physics, Faculty of Sciences, Gazi University, 06500, Teknikokullar, Ankara, Turkey |
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| Abstract: | Electrochemical water splitting to hydrogen is considered as a promising approach for clean H2 production. However, developing highly active and inexpensive electrocatalysts is an important part of the hydrogen evolution reaction (HER). Herein, we present a multifaceted atom (sp2-and sp-hybridized boron) doping strategy to directly fine-modify the electronic structures of the active site and the HER performance by the density functional theory calculations. It is found that the binding strength between the Co atom and the B doped graphyne nanosheets can be enhanced by doping B atoms. Meanwhile, the Co@B1-GY and Co@B2-GY catalysts exhibit good thermodynamic stability and high HER catalytic activity. Interestingly, the Co@B2-GY catalyst has an ideal HER performance with the ΔGH* value of ?0.004 eV. Moreover, the d-band center of the Co atoms is upshifted by the sp2-or sp-hybridized B dopants. The concentrations of the sp-hybridized B atoms have a positive effect on the electrons transformation of the Co atoms. The interaction between the H and Co atoms becomes strong with the increase of the concentrations of the sp-hybridized B atoms and thus the corresponding catalysts show sluggish HER kinetics. This investigation could provide useful guidance for the experimental groups to directly and continuously control the catalytic activity towards HER by precisely doping multifaceted atoms. |
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| Keywords: | Doping B atom Graphyne Single-atom catalysts Hydrogen evolution reaction Density functional theory |
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