Boosted CO desorption behaviors induced by spatial dyadic heterostructure in polymeric carbon nitride for efficient photocatalytic CO2 conversion

Abstract

In the present contribution, a highly crystalline nano-coral matrix on amorphous polymeric carbon nitride (PCN) nanosheets are structurally crafted and identified as an efficient photocatalyst for photocatalytic CO2 reduction reaction (CRR). The modified PCN presents a unique spatial dyadic heterostructure and favorable directional charge-transfer channel, resulting in improved charge separation for CRR. Notably, DFT calculations suggest that the modified PCN possesses reduced energy barrier for CO2 reduction into CO via facile accessible of COOH intermediate and boosted CO* desorption. The as-prepared functionalized PCN materials possess a remarkable photocatalytic CO2 reduction performance, yielding CO at a rate of 486.7 μmol h−1 g−1 (i.e. 34.0 folds’ higher than pristine PCN) with a high selectivity of 98.4 %. Our strategy of designing spatial dyadic heterostructure in polymeric carbon nitride provides new insights into the architecture engineering of CRR photocatalysts for efficient CO desorption and CO2 conversion.