Industrial-Level CO2 Electroreduction Using Solid-Electrolyte Devices Enabled by High-Loading Nickel Atomic Site Catalysts

Transition-metal atomic site catalysts (ASCs) are a new class of catalytic system for CO2 electroreduction, however, their practical application is greatly hindered by the challenge that it's still difficult for them to simultaneously achieve industrial-level current density and high selectivity. Herein a new strategy is reported for hundreds of gram-scale and low-cost production of Ni-ASCs on 3D porous nanocarbon with high-loading Ni-N-3 sites for greatly boosting the electroreduction of CO2 to CO with both industrial-level current density and high selectivity. It is discovered that although Ni-ASCs with high-loading (Ni-ASCs/4.3 wt.%) and low-loading (Ni-ASCs/0.8 wt.%) both show above 95% Faradic efficiency for CO (FECO) under a wide potential range in H-cell, in flow cell, Ni-ASCs/0.8 wt.% can only achieve FECO of 43.6% at a current density of 343.9 mA cm(-2), significantly lower than those (95.1%, 533.3 mA cm(-2)) of Ni-ASCs/4.3 wt.% under same potential, first revealing the important role of high-loadings of single atom sites in promoting the high-selectivity electrolysis at industrial-level current density. Most importantly, it is demonstrated that Ni-ASCs/4.3 wt.%-based membrane electrode assembly (MEA) exhibits outstanding durability at industrial-level current density of 360.0 mA cm(-2), which is one of the best performances for the realistic electroreduction of CO2 to CO in the reported ASCs-based MEA systems.