Chen Yan, Li Ao, Fu Xiuli, Peng Zhijian
School of Science, China University of Geosciences, Beijing 100083, China.
School of Science, Beijing University of Posts and Telecommunications, Beijing 100876, China.
Molecules. 2022 Oct 24;27(21):7178. doi: 10.3390/molecules27217178.
The difficulty of exposing active sites and easy recombination of photogenerated carriers have always been two critical problems restricting the photocatalytic activity of g-CN. Herein, a simple (NH)MoO-induced one-step calcination method was successfully introduced to transform bulk g-CN into g-CN/MoO composites with a large specific surface area. During the calcination, with the assistance of NH and water vapor produced by ammonium molybdate, the pyrolytical oxidation and depolymerization of a g-CN interlayer were accelerated, finally realizing the exfoliation of the g-CN. Furthermore, another pyrolytical product of ammonium molybdate was transformed into MoO under an NH atmosphere, which was in situ loaded on the surface of a g-CN nanosheet. Additionally, the results of photocatalytic hydrogen evolution under visible light show that the optimal g-CN/MoO composite has a high specific surface area and much improved performance, which is 4.1 times that of pure bulk g-CN. Such performance improvement can be attributed to the full exposure of active sites and the formation of abundant heterojunctions. However, with an increasing feed amount of ammonium molybdate, the oxidation degree of g-CN was enhanced, which would widen the band gap of g-CN, leading to a weaker response ability to visible light. The present strategy will provide a new idea for the simple realization of exfoliation and constructing a heterojunction for g-CN simultaneously.
暴露活性位点的困难以及光生载流子的容易复合一直是限制g-CN光催化活性的两个关键问题。在此,成功引入了一种简单的(NH)MoO诱导一步煅烧方法,将块状g-CN转化为具有大比表面积的g-CN/MoO复合材料。在煅烧过程中,在钼酸铵产生的NH和水蒸气的辅助下,g-CN层间的热解氧化和解聚加速,最终实现了g-CN的剥离。此外,钼酸铵的另一种热解产物在NH气氛下转化为MoO,并原位负载在g-CN纳米片的表面。另外,可见光下光催化析氢的结果表明,最佳的g-CN/MoO复合材料具有高比表面积和大大提高的性能,是纯块状g-CN的4.1倍。这种性能的提高可归因于活性位点的充分暴露和大量异质结的形成。然而,随着钼酸铵进料量的增加,g-CN的氧化程度增强,这将拓宽g-CN的带隙,导致对可见光的响应能力减弱。本策略将为简单实现g-CN的剥离并同时构建异质结提供新思路。