Matched Redox Kinetics on Triazine‐Based Carbon Nitride/Ni(OH)2 for Stoichiometric Overall Photocatalytic CO2 Conversion

Abstract Mismatched reaction kinetics of CO 2 reduction and H 2 O oxidation is the main obstacle limiting the overall photocatalytic CO 2 conversion. Here, a molten salt strategy is used to construct tubular triazine‐based carbon nitride (TCN) with more adsorption sites and stronger activation capability. Ni(OH) 2 nanosheets are then grown over the TCN to trigger a proton‐coupled electron transfer for a stoichiometric overall photocatalytic CO 2 conversion via “3CO 2 + 2H 2 O = CH 4 + 2CO + 3O 2 .” TCN reduces the energy barrier of H 2 O dissociation to promote H 2 O oxidation to O 2 and supply sufficient protons to Ni(OH) 2 , whereby the CO 2 conversion is accelerated due to the enhanced proton‐coupled electron transfer process enabled by the sufficient proton supply from TCN. This work highlights the importance of matching the reaction kinetics of CO 2 reduction and H 2 O oxidation by proton‐coupled electron transfer on stoichiometric overall photocatalytic CO 2 conversion.