American Chemical Society
nn4c03922_si_001.pdf (1.35 MB)

Supercritical CH3OH-Triggered Isotype Heterojunction and Groups in g‑C3N4 for Enhanced Photocatalytic H2 Evolution

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journal contribution
posted on 2024-05-16, 02:33 authored by Liuhao Mao, Binjiang Zhai, Jinwen Shi, Xing Kang, Bingru Lu, Yanbing Liu, Cheng Cheng, Hui Jin, Eric Lichtfouse, Liejin Guo
The structure tuning of bulk graphitic carbon nitride (g-C3N4) is a critical way to promote the charge carriers dynamics for enhancing photocatalytic H2-evolution activity. Exploring feasible post-treatment strategies can lead to effective structure tuning, but it still remains a great challenge. Herein, a supercritical CH3OH (ScMeOH) post-treatment strategy (250–300 °C, 8.1–11.8 MPa) is developed for the structure tuning of bulk g-C3N4. This strategy presented advantages of time-saving (less than 10 min), high yield (over 80%), and scalability due to the enhanced mass transfer and high reactivity of ScMeOH. During the ScMeOH post-treatment process, CH3OH molecules diffused into the interlayers of g-C3N4 and subsequently participated in N-methylation and hydroxylation reactions with the intralayers, resulting in a partial phase transformation from g-C3N4 into carbon nitride with a poly­(heptazine imide)-like structure (Q-PHI) as well as abundant methyl and hydroxyl groups. The modified g-C3N4 showed enhanced photocatalytic activity with an H2-evolution rate 7.2 times that of pristine g-C3N4, which was attributed to the synergistic effects of the g-C3N4/Q-PHI isotype heterojunction construction, group modulation, and surface area increase. This work presents a post-treatment strategy for structure tuning of bulk g-C3N4 and serves as a case for the application of supercritical fluid technology in photocatalyst synthesis.