Single boron atom anchored on graphitic carbon nitride nanosheet(B/g-C_(2)N)as a photocatalyst for nitrogen fixation:A first-principles study

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.