Single-atomic-Ni electrocatalyst derived from phthalocyanine-modified MOF for convoying CO2 intelligent utilization

Abstract

Single-atomic-site catalysts have been demonstrated as promising candidates for electrochemical CO2 reduction reaction (eCO2RR). However, the universal construction strategies need to be further developed to synthesize the desired single-atomic-site catalysts with high eCO2RR activity for feasible CO2 utilization. Herein, a novel 2-methylimidazole-phthalocyanine-Ni (IM4NiPc) coordinatively modified ZIF-8 was rationally fabricated and applied to derive the single-atomic-Ni electrocatalyst (Ni-N-C-l), which is capable of delivering much improved activity for eCO2RR, compared to the pristine IM4NiPc immobilized onto ZIF-8-derived N-doped carbon surface, and is also comparable to the best reported catalysts. The satisfied Faradaic efficiency, current density and stability of CO2-to-CO electroconversion over Ni-N-C-l are shown to originate from the verified Ni-N4 configuration, particularly, reaching a CO Faradaic efficiency of 99% in a wide potential range. Moreover, based on the outstanding eCO2RR activity of Ni-N-C-l, we successfully realized the exemplary synthesis of amide polymer materials through CO-mediated electro/thermocatalytic cascade processes, demonstrating the feasibility of utilizing CO2 for material manufacturing. This finding is expected to provide useful insight on the precise design and rational synthesis of the novel single-atomic-site catalysts for future CO2 intelligent utilization.