Frustrated Lewis Pairs Constructed on 2D Amorphous Carbon Nitride for High-Selective Photocatalytic CO2 Reduction to CH4

Photocatalytic reduction of CO2 into high value-added fuels paves a new avenue for alleviating the energy crisis and green-house effect, yet it is still challenging to achieve a highly active photocatalyst with high selectivity. Herein, for the first time, a facile structural engineering strategy is developed to construct tunable frustrated Lewis pairs (FLPs) on 2D amorphous graphitic carbon nitride (C3N4) via the introduction of boric acid with the assistance of supercritical CO2, wherein the FLPs are composed of -B(OH)(2) groups (Lewis acid sites) and adjacent -NHx (Lewis base sites). Ideally, the synergetic effects of the FLPs on the 2D amorphous C3N4 can help to efficiently adsorb, activate, and reduce CO2 to CH4 with enhanced selectivity of approximate to 96.0%.