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Understanding the Efficiency and Selectivity of Two-Electron Production of Metalloporphyrin-Embedded Zirconium-Pyrogallol Scaffolds in Electrochemical CO2 Reduction.

Because of the high efficiency and mild reaction conditions, electrocatalytic CO2 reduction (ECR) has attracted significant attention in recent years. However, the specific mechanism of the formation of the two-electron production (CO or HCOOH) in this reaction is still unclear. Herein, with density functional theory calculation and experimental manipulation, the specific mechanism of the selective two-electron reduction of CO2 has been systematically investigated, employing the polyphenolate-substituted metalloporphyrinic frameworks, ZrPP-1-M (M = Fe, Co, Ni, Cu, and Zn), as model catalysts. Experimental observations and theoretical calculations discovered that ZrPP-1-Co is a more favorable catalyst for ECR among them. Compared with the formation of HCOOH, electroreduction of CO2 into CO has more beneficial thermodynamic and kinetic routes with ZrPP-1-Co as a catalyst. After introducing the r-GO for improving the conductivity, the Faradaic efficiency for CO formation is 82.4% at -0.6 v (vs RHE).