Theoretical Study on Electroreduction of CO2 to C3+ Catalyzed by Polymetallic Phthalocyanine Covalent Organic Frameworks (COFs) in Tandem

In CO2RR, CO2 can be changed into a wide succession of premium chemicals and fuels, amid which C3+ products such as n-propanol, n-propanol is of great economic value. To improve the selectivity of C-3 products, the idea of tandem catalysis is proposed in this paper through the reduction of CO2 to CO, followed by the electrochemical reduction reaction of CO to n-propanol, we screen out Fe-Co-Pc-Ni-O-COFs catalyst that was the most promising catalyst by DFT calculation method, NiO4 and Fe-Co-Pc can work independently that the CO generated on NiO4 can spontaneously and rapidly migrate to the active sites of Fe-Co-Pc catalyst that C-1-C-1 coupling can be carried out to obtain C-2 intermediates and C-2 intermediates can be coupled with CO (C-1-C-2 coupling) to obtain C-3 products. Finally, it is concluded that *CO-*CHO coupling is the most critical steps in the formation of C-2 products, the coupling of *CH3CHO with *CO to form *CH3CHOCO is a key step to generate the n-propanol, an optimal way to form C-3 is also screened out. [GRAPHICS] .