Micro-tailored g-C3N4 enables Ru single-atom loading for efficient photocatalytic H2 evolution,Applied Surface Science

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Micro-tailored g-C3N4 enables Ru single-atom loading for efficient photocatalytic H2 evolution
Applied Surface Science ( IF 6.3 ) Pub Date : 2022-04-29 , DOI: 10.1016/j.apsusc.2022.153471
Chengjie Li _{1,

2} , Xiqing Dong ₁ , Yingchao Zhang ₁ , Jing Hu ₁ , Jinxiu Yuan ₁ , Guofu Li ₁ , Di Chen ₁ , Yuning Li ₃

Affiliation

Loading single atom (SA) cocatalysts onto semiconductors offers great potential for improving the photocatalytic performance. Here, we report a simple micro-tailoring strategy that cuts g-C3N4 into small pieces and oligomers. Defects, boundaries, dopants and terminal groups created could confine Ru SAs stably onto the framework, ensuring uniform dispersion of Ru SAs on the tailored g-C3N4. The as-prepared composite, the tailored g-C3N4 loaded with Ru SAs, showed a dramatic increase photocatalytic activity for H2 evolution (4052.1 μmol h−1 g−1) compared to the composite of the non-tailored g-C3N4 loaded with Ru (394.3 μmol h−1 g−1). The enhanced catalytic activity was achieved by the metal-support interaction between the Ru atoms and the tailored g-C3N4, which could manipulate local charge distribution, thus promoting the adsorption of intermediates and enabling efficient charge transfer. In addition, atomic Ru-sites could provide directional charge transfer channels and targeting sites to facilitate rapid photo-introduced charge transfer and water reduction reaction. The proposed strategy provides a facile and feasible way for the construction of atomically dispersed catalysts for efficient photocatalytic H2 evolution and other reactions.

中文翻译：

微定制 g-C3N4 可实现 Ru 单原子负载，实现高效的光催化 H2 析出

将单原子（SA）助催化剂负载到半导体上为提高光催化性能提供了巨大的潜力。在这里，我们报道了一种简单的微定制策略，该策略将 g-C3N4 切割成小块和低聚物。产生的缺陷、边界、掺杂剂和末端基团可以将 Ru SAs 稳定地限制在框架上，确保 Ru SAs 在定制的 g-C3N4 上均匀分散。与负载 Ru 的非定制 g-C3N4 的复合材料（394.3 μmol h-1 g-1）相比，所制备的复合材料，即负载 Ru SA 的定制 g-C3N4 显示出显着增加的 H2 析出光催化活性（4052.1 μmol h-1 g-1）。增强的催化活性是通过 Ru 原子和定制的 g-C3N4 之间的金属载体相互作用实现的，它可以操纵局部电荷分布，从而促进中间体的吸附并实现高效的电荷转移。此外，原子 Ru 位点可以提供定向电荷转移通道和靶向位点，以促进快速光引入电荷转移和水还原反应。所提出的策略为构建原子分散催化剂提供了一种简单可行的途径，用于高效的光催化 H2 析出和其他反应。

更新日期：2022-04-29

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