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.
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