Homogeneous Carbon/Potassium-Incorporation Strategy for Synthesizing Red Polymeric Carbon Nitride Capable of Near-Infrared Photocatalytic H2 Production.

Abstract

The efficient utilization of near-infrared (NIR) light for photocatalytic hydrogen generation is vitally important to both solar hydrogen energy and hydrogen medicine, but remains a challenge at present, owing to the strict requirement of the semiconductor for high NIR responsiveness, narrow bandgap, and suitable redox potentials. Here, an NIR-active carbon/potassium-doped red polymeric carbon nitride (RPCN) is achieved for by using a similar-structure dopant as the melamine (C3 H6 N6 ) precursor with the solid KCl. The homogeneous and high incorporation of carbon and potassium remarkably narrows the bandgap of carbon nitride (1.7eV) and endows RPCN with a high NIR-photocatalytic activity for H2 evolution from water at the rate of 140 µmol h-1 g-1 under NIR irradiation (700 nm ≤ λ≤ 780nm), and the apparent quantum efficiency is high as 0.84% at 700 ± 10nm (and 13% at 500 ± 10nm). A proof-of-concept experiment on a tumor-bearing mouse model verifies RPCN as being capable of intratumoral NIR-photocatalytic hydrogen generation and simultaneous glutathione deprivation for safe and high-efficacy drug-free cancer therapy. The results shed light on designing efficient photocatalysts to capture the full spectrum of solar energy, and also pioneer a new pathway to develop NIR photocatalysts for hydrogen therapy of major diseases.