中国物理B ›› 2021, Vol. 30 ›› Issue (8): 83101-083101.doi: 10.1088/1674-1056/abe3f6

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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. 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
  • 收稿日期:2020-12-24 修回日期:2021-02-04 接受日期:2021-02-08 出版日期:2021-07-16 发布日期:2021-07-16
  • 通讯作者: Shi-Hao Wei E-mail:weishihao@nbu.edu.cn
  • 基金资助:
    Project supported by the National Natural Science Foundation of China (Grant No. 51871126) and the K. C. Wong Magna Fund in Ningbo University.

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. 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
  • Received:2020-12-24 Revised:2021-02-04 Accepted:2021-02-08 Online:2021-07-16 Published:2021-07-16
  • Contact: Shi-Hao Wei E-mail:weishihao@nbu.edu.cn
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Grant No. 51871126) and the K. C. Wong Magna Fund in Ningbo University.

摘要: 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.

关键词: first-principles calculation, N2 reduction, catalysts, electronic structure, reaction mechanisms, reaction paths

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.

Key words: first-principles calculation, N2 reduction, catalysts, electronic structure, reaction mechanisms, reaction paths

中图分类号:  (Ab initio calculations)

  • 31.15.A-
34.70.+e (Charge transfer) 73.22.-f (Electronic structure of nanoscale materials and related systems) 82.20.Kh (Potential energy surfaces for chemical reactions)