Regulating coordination environment of main-group elements co-doped graphene: Boost CO2RR activity

As a catalyst, the coordination environment of the doped main group elements in graphene directly affects the carbon dioxide reduction reaction (CO 2 RR) activity. For the elements (Ga, Ge, As, Sn, Sb and Bi) and N/B/P/S codoped graphene, we systematically investigated the effect of coordination environment on the performance of catalytic CO 2 RR. Compared with B 4 coordination, N 4 counterpart co -doped main group element system is more stable and exhibits better performance as catalysts. For N 4 -based catalysts asymmetrically substituting with B, P or S, the charge distribution around the active center is polarized, which results in the lower limiting potential of CO 2 RR. In particular, with Sb as the catalytic center, the U L decreased from - 0.8 V (Sb-N 4 ) and - 1.6 V (Sb-B 4 ) to - 0.63 V (Sb-N 3 S). Moreover, in the Bi-N 4 system, the substitution of one S atom with one N atom could control the reaction products (formic acid or methane), which provides a novel strategy for the selective generation of CO 2 RR products.