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

Photocatalytic reduction of CO 2 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 (C 3 N 4 ) via the introduction of boric acid with the assistance of supercritical CO 2 , wherein the FLPs are composed of B(OH) 2 groups (Lewis acid sites) and adjacent NH x (Lewis base sites). Ideally, the synergetic effects of the FLPs on the 2D amorphous C 3 N 4 can help to efficiently adsorb, activate, and reduce CO 2 to CH 4 with enhanced selectivity of ≈96.0%.