Abstract
Based on the experimentally reported stable and conductive two-dimensional covalent organic frameworks with copper phthalocyanine (CuPc) as building block and cyan substituted phenyl as connector (CuCOF-CN) as an electrocatalyst for CO(2) reduction reaction (RR), first principle calculations were performed on CuCOF-CN and its analog with the CN being replaced by H (CuCOF). Comparatively studied on the crystal structures, electronic properties, and CO(2)RR performance of the two catalysts found that CuCOF has reduced crystal unit size, more positive charge on Cu and CuPc segments, smaller band gap, and lower reaction barrier for CO(2) RR than CuCOF-CN. CuCOF is proposed to be good potential electrocatalyst with good environment friendliness. The substituent effect and structure-property-performance relationship would help for designing and fabricating new electrocatalysts.