Adjusting Surface Oxidized Layer of CoTe on PCN via In Situ N-Doping Strategy to Promote Charge Separation of Z-Scheme Heterojunction for Propelling Photocatalytic CO2 Reduction.

Abstract

It has been a challenging issue to profoundly actuate the transfer and separation of photoinduced charge carriers by controlling the interface structure inside the heterojunction, owing to the molecular/subnanometric level interface region. Herein, a unique one-dimensional/two-dimensional (1D/2D) CoTe/PCN Z-scheme heterojunction is fabricated through the self-assembly of CoTe nanorods on the surface of polymeric carbon nitride (PCN) nanosheets. Significantly, in situ N-doping in the molecular/subnanometric surface oxidized layer of CoTe nanorods is achieved, effectively adjusting its chemical structure and element chemical states. Moreover, this N-doped surface oxidized layer can serve as a recombination region of photogenerated electrons from PCN and photogenerated holes from CoTe to increase the overall carrier separation efficiency in the Z-scheme heterojunction actuated by the built-in electric field. As a result, the photocatalytic CO2 reduction (CO2R) performance is enhanced dramatically, in which the yield of CO generated over the optimal 1D/2D CoTe/PCN heterojunction reaches up to triple than that over PCN. This unique contribution provides an emblematic paradigm for adjusting the interfacial structure of heterojunction and has a profound insight into the interfacial adjusting mechanism to improve the charge separation efficiency in the photocatalytic reaction.