Large-Scale and Highly Selective CO2 Electrocatalytic Reduction on Nickel Single-Atom Catalyst

Summary The scaling up of electrocatalytic CO 2 reduction for practical applications is still hindered by a few challenges: low selectivity, small current density to maintain a reasonable selectivity, and the cost of the catalytic materials. Here we report a facile synthesis of earth-abundant Ni single-atom catalysts on commercial carbon black, which were further employed in a gas-phase electrocatalytic reactor under ambient conditions. As a result, those single-atomic sites exhibit an extraordinary performance in reducing CO 2 to CO, yielding a current density above 100 mA cm −2 , with nearly 100% selectivity for CO and around 1% toward the hydrogen evolution side reaction. By further scaling up the electrode into a 10 × 10-cm 2 modular cell, the overall current in one unit cell can easily ramp up to more than 8 A while maintaining an exclusive CO evolution with a generation rate of 3.34 L hr −1 per unit cell.