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.

Keywords

Single-atomic-site catalysts / electrochemical CO₂ reduction reaction / electro/thermocatalytic cascade process / amide polymers

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