An imidazolate framework-derived single-atom nickel catalyst for the reduction of CO2 to CO†

Abstract

The reduction of carbon dioxide (CO₂) using electrochemical methods is one of the ways to achieve carbon recycling, as the increase in carbon dioxide emissions causes environmental problems. Single-atom dispersed Ni-NC site catalysts have emerged as effective electrocatalysts for the reduction of CO₂ to CO. Using ZIF-8 as a carrier, we aim to design a high-performance single nickel-site catalyst by elucidating the structure evolution of NiN_x sites during thermal activation as well as other key external factors such as the carbon particle size and nickel content. The pyridine N active sites generated after calcination have higher activity and CO selectivity. The catalyst achieved up to 99.6% CO generation at −0.88 V vs. RHE, and is one of the best catalysts for the reduction of CO₂ to CO. This work demonstrates an effective method for designing efficient electrochemical CO₂ reduction catalysts by tuning the surface structure of single-atom anchored carriers.