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Abstract

Summary
Polymeric carbon nitrides (CNs) are regarded as the most sustainable materials for solar energy conversion via photocatalytic processes.
However, the first-generation CNs suffered from imperfect charge separation and insufficient CO₂ adsorption.
Herein, the construction of a heterojunction material involving highly crystalline CN-nanorods with ordered alignment on graphene is delineated, which improves light harvesting, CO₂ capture, and interface charge transfer.
The graphene-supported 1D nano-arrays of crystalline CNs show a comparably high selectivity of CO₂/N2 up to 44, with an isosteric heat of adsorption of 55.2 kJ/mol for CO₂.
The heterojunction material also drives the simple and efficient CO₂ photoreduction in the gas phase, without the addition of any cocatalyst or sacrificial agent, even at the more relevant case of low concentrations of CO₂.
These findings provide a robust way for tailoring the performance of CN materials, with the aim of a practicable technological application for CO₂ capture and photoreduction.