MOF-Derived Ni Single-Atom Catalyst with Abundant Mesopores for Efficient Mass Transport in Electrolytic Bicarbonate Conversion

Direct electrolytic CO₂ capture solution (e.g., bicarbonate), which bypasses the energy-intensive processes of CO₂ desorption, offers a unique route for CO₂ conversion to fuels or value-added chemicals. Nonprecious Ni single-atom catalysts (SACs) anchored on metal-organic frameworks (MOFs) possess abundant porous structures and exhibit a high selectivity for CO production. However, these MOF-derived Ni SACs are usually synthesized by a series of complex procedures, and their abundant micropores (<2 nm) also reduce the local reactant transport in the catalysts. Herein, we report a simple one-step pyrolysis method to prepare a MOF-derived Ni SAC that can efficiently boost bicarbonate conversion to CO. The abundant mesopores around 35.4 nm significantly enhance the transport of local reactants in the catalysts. At a high current density of 100 mA/cm², the tailored catalyst shows 67.2% Faradaic efficiency of CO, which, to the best of our knowledge, exceeds the state-of-the-art precious Ag nanoparticle catalysts reported so far. This study highlights the significance of developing nonprecious catalysts for employment in large-scale bicarbonate electrolysis conversion devices.