Atomically Dispersed Nickel Sites for Selective Electroreduction of CO₂

Abstract

Electrocatalytic CO2 reduction at its point of generation to form fuels and commodity chemicals using electricity from renewable sources is an appealing strategy for decreasing net anthropogenic CO2 emissions and mitigating global warming. CO2 reduction is however a kinetically slow and energy intensive reaction with a wide range of possible products. Therefore, the development of highly selective, energy-efficient, and cost-effective electrocatalysts is required to accelerate this kinetically sluggish process. We report facile synthesis of atomically dispersed Ni sites supported on nitrogen-doped carbon (Ni/NC), which significantly facilitates selective electrochemical CO2 reduction to CO with a Faradaic efficiency reaching 92.3% at a low overpotential of 0.69 V (relative to the formal redox potential of CO2 reduction to CO, E0redox = −0.11 V versus reversible hydrogen electrode, pH 0), surpassing Ni particles and many other reported metal-based catalysts. This study thus unveils a platform of activating Ni sites for selective reduction of CO2.