Design and catalytic performance investigation of the Ni–N–C catalyst for CO2RR: a theoretical study†

The combustion of fossil fuels is increasingly contributing to global warming. The recycling of CO₂ plays a crucial role, and the creation of a highly efficient electrocatalyst is essential for enhancing the efficiency of the reaction. This work focused on the theoretical design of Ni–N–C catalysts with different coordination environments of Ni through quantum chemical calculations and analyzed the differences between the coordination environments of pyridine N and pyrrole N on the performance of catalytic CO₂ reduction to CO in order to identify the most efficient catalyst configuration. The Ni–N bonding energy of the catalyst with a vacancy was greater than that of the catalyst without a vacancy, and the activation ability of Ni-pyridine N₂C₁–C was the best. Ultimately, examining various catalysts for converting CO₂ into CO revealed that Ni-pyridine N₂C₁–C exhibited the most effective catalytic impact. In contrast to the energy barrier ΔG = 2.9903 eV in the absence of a catalyst, the energy barrier ΔG = −1.4029 eV during the CO₂ to CO catalytic reaction decreased by 4.3932 eV. This decrease was the largest among all the catalysts mentioned above, and the reaction could be spontaneous from a thermodynamic perspective. The research results provide a theoretical reference for the experimental preparation of catalysts for CO₂ to CO conversion and the resource utilization of CO₂.