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-C_(2)N can serve as high performance photocatalyst in N_(2)fixation,where single boron atom is anchored on the g-C_(2)N to form B/g-C_(2)N.With the introduction of B atom to g-C_(2)N,the energy gap reduces from 2.45 eV to 1.21 eV and shows strong absorption in the visible light region.In addition,N_(2)can be efficiently reduced on B/g-C_(2)N 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-C_(2)N and N_(2)plays a key role to active N_(2),and the BN_(2)moiety of B/g-C_(2)N acts as active and transportation center.The activity originates from the strong interaction between 1π1π*orbitals of N_(2)and molecular orbitals of B/g-C_(2)N,the ionization of 1πorbital and the filling of 1π*orbital can increase the N≡N bond length greatly,making the activation of N_(2).Overall,this work demonstrates that B/g-C_(2)N is a promising photocatalyst for N_(2)fixation.
作者
Hao-Ran Zhu
Jia-Liang Chen
Shi-Hao Wei
祝浩然;陈嘉亮;韦世豪(Department of Microelectronic Science and Engineering,School of Physical Science and Technology,Ningbo University,Ningbo 315211,China;College of Electronic Information and Optical Engineering,Nankai University,Tianjin 300350,China)
基金
Project supported by the National Natural Science Foundation of China (Grant No. 51871126)
the K. C. Wong Magna Fund in Ningbo University
