潍坊学院姜在勇团队报道了g-C₃N₄ S型同质结通过范德华界面调节的本征聚合调整，增强光催化析氢和CO₂还原。相关研究成果于2025年1月9日发表在国际顶尖学术期刊《德国应用化学》。

有效的S型同质结依赖于能带结构的精确调节，和有利电荷迁移界面的构建。

该文中，研究人员通过自组装超分子前体的精细聚合来调节g-C₃N₄的电子结构性质。实验和DFT结果表明，本征带隙和表面电子特性都得到了调整，导致在本征范德华力的作用下形成了原位重建的同质结界面。由g-C₃N₄纳米点和超薄g-C₃N₄纳米粒子组成的同质结催化剂表现出显著的S型载流子分离机制，提高了电子和空穴的利用率。因此，在AM 1.5光照（~100 mW/cm²）下，g-C₃N₄同质结光催化剂实现了580μmol h^-1的显著析氢速率。

此外，在CO₂还原中观察到CH₄选择性的逆转，产生80.30μmol g^-1 h^-1，选择性为96.86%，而块状g-C₃N₄的性能仅产生2.22μmol g^-1 h^-1，CH₄选择性为15.69%。这些发现不仅突显了g-C₃N₄同质结光催化剂在氢气生产和二氧化碳减排方面的巨大潜力，还为优化g-C₃N₄的结构特性提出了一种优越有效的策略，这对光催化反应的设计至关重要。

附：英文原文

Title: g-C3N4 S-Scheme Homojunction through van der Waals Interface Regulation by Intrinsic Polymerization Tailoring for Enhanced Photocatalytic H2 Evolution and CO2 Reduction

Author: Xianglin Zhu, Enlong Zhou, Xishi Tai, Huibin Zong, Jianjian Yi, Zhimin Yuan, Xingling Zhao, Peng Huang, Hui Xu, Zaiyong Jiang

Issue&Volume: 2025-01-09

Abstract: The effective S-scheme homojunction relies on the precise regulation of band structure and construction of advantaged charge migration interfaces. Here, the electronic structural properties of g-C3N4 were modulated through meticulous polymerization of self-assembled supramolecular precursors. Experimental and DFT results indicate that both the intrinsic bandgap and surface electronic characteristics were adjusted, leading to the formation of an in-situ reconstructed homojunction interface facilitated by intrinsic van der Waals forces. The homojunction catalyst, composed of g-C3N4 nanodots and ultra-thin g-C3N4 nanoflakes, exhibited a significant S-scheme carrier separation mechanism, which enhances the utilization of electrons and holes. Consequently, under AM 1.5 light irradiation (~100 mW/cm2), the g-C3N4 homojunction photocatalyst achieved a remarkable hydrogen evolution rate of 580 μmol h-1. Furthermore, a reversed CH4 selectivity in CO2 reduction was observed, yielding 80.30 μmol g1 h1 with a selectivity of 96.86%, in contrast to the performance of bulk g-C3N4, which produced only 2.22 μmol g1 h1 with the 15.69% CH4 selectivity. These findings not only highlight the significant potential of the g-C3N4 homojunction photocatalyst for hydrogen production and CO2 reduction but also propose a superior and effective strategy for optimizing the structural properties of g-C3N4, which are crucial for the design of photocatalytic reactions.

DOI: 10.1002/anie.202425439

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202425439