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Single boron atom anchored on graphitic carbon nitride nanosheet (B/g-C2N) as a photocatalyst for nitrogen fixation: A first-principles study |
| Hao-Ran Zhu(祝浩然)1,2, Jia-Liang Chen(陈嘉亮)1, and Shi-Hao Wei(韦世豪)1,† |
1 Department of Microelectronic Science and Engineering, School of Physical Science and Technology, Ningbo University, Ningbo 315211, China;
2 College of Electronic Information and Optical Engineering, Nankai University, Tianjin 300350, China |
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Abstract It is essential to explore high efficient catalysts for nitrogen reduction in ammonia production. Based on the first-principles calculation, we find that B/g-C2N can serve as high performance photocatalyst in N2 fixation, where single boron atom is anchored on the g-C2N to form B/g-C2N. With the introduction of B atom to g-C2N, the energy gap reduces from 2.45 eV to 1.21 eV and shows strong absorption in the visible light region. In addition, N2 can be efficiently reduced on B/g-C2N through the enzymatic mechanism with low onset potential of 0.07 V and rate-determining barrier of 0.50 eV. The "acceptance-donation" interaction between B/g-C2N and N2 plays a key role to active N2, and the BN2 moiety of B/g-C2N acts as active and transportation center. The activity originates from the strong interaction between 1π1π* orbitals of N2 and molecular orbitals of B/g-C2N, the ionization of 1π orbital and the filling of 1π* orbital can increase the N≡N bond length greatly, making the activation of N2. Overall, this work demonstrates that B/g-C2N is a promising photocatalyst for N2 fixation.
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Received: 24 December 2020
Revised: 04 February 2021
Accepted manuscript online: 08 February 2021
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PACS:
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31.15.A-
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(Ab initio calculations)
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34.70.+e
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(Charge transfer)
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73.22.-f
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(Electronic structure of nanoscale materials and related systems)
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82.20.Kh
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(Potential energy surfaces for chemical reactions)
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| Fund: Project supported by the National Natural Science Foundation of China (Grant No. 51871126) and the K. C. Wong Magna Fund in Ningbo University. |
Corresponding Authors:
Shi-Hao Wei
E-mail: weishihao@nbu.edu.cn
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Cite this article:
Hao-Ran Zhu(祝浩然), Jia-Liang Chen(陈嘉亮), and Shi-Hao Wei(韦世豪) Single boron atom anchored on graphitic carbon nitride nanosheet (B/g-C2N) as a photocatalyst for nitrogen fixation: A first-principles study 2021 Chin. Phys. B 30 083101
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