Faculty of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, PR China.
Department of Chemistry, College of Science, Shantou University, Shantou, Guangdong 515063, PR China.
J Colloid Interface Sci. 2022 Jan 15;606(Pt 2):1311-1321. doi: 10.1016/j.jcis.2021.08.176. Epub 2021 Aug 28.
Constructing noble metal-doped g-CN/carbon composites is a feasible route to overcome the intrinsic drawbacks of pristine g-CN for enhanced activity of CO photoreduction. Herein, a novel Ag-doped g-CN/biomass-derived carbon composite with hollow bird's nest-like (Ag-g-CN/BN-C) is designed and prepared via a simple yet effective one-step pyrolysis method. In the Ag-g-CN/BN-C, the highly-dispersed Ag nanoparticles (20-30 nm) with the surface plasmon resonance (SPR) effect act as a significant cocatalyst not only to efficiently trap the photogenerated electrons from g-CN to boost the separation of photogenerated electron-hole pairs but also to produce additional active "hot electrons", while the conductive quasi-spherical hollow structure of BN-C doubles the specific surface area with multiple reflections of light, providing abundant active sites and more utilization efficiency of light energy. As a result, the Ag-g-CN/BN-C exhibits a remarkably enhanced CO evolution rate of 33.3 μmol·g·h without addition of any sacrificial reagents and photosensitizers, superior to those of both the pristine g-CN and many reported g-CN-based counterparts. The findings of this work demonstrate a good indication for integrating g-CN with SPR-dependence noble metal and renewable biomass-derived carbon for enhanced CO photoreduction, which may be extended to modify other semiconductor materials for more photocatalytic applications with enhanced activity.
构建贵金属掺杂 g-CN/碳复合材料是克服原始 g-CN 固有缺陷、提高 CO 光还原活性的可行途径。在此,通过一种简单而有效的一步热解法,设计并制备了一种新型的 Ag 掺杂 g-CN/生物质衍生碳复合材料,具有空心鸟巢状结构(Ag-g-CN/BN-C)。在 Ag-g-CN/BN-C 中,具有表面等离子体共振(SPR)效应的高分散 Ag 纳米粒子(20-30nm)不仅可以作为有效的助催化剂,有效地从 g-CN 中捕获光生电子,从而促进光生电子空穴对的分离,而且还可以产生额外的活性“热电子”,而 BN-C 的导电类球形空心结构使比表面积加倍,并实现多次光反射,提供丰富的活性位点和更高的光能利用率。结果表明,Ag-g-CN/BN-C 在不添加任何牺牲剂和光敏剂的情况下,CO 演化速率达到 33.3μmol·g·h-1,明显优于原始 g-CN 和许多报道的 g-CN 基复合材料。这项工作的发现表明,将 g-CN 与依赖 SPR 的贵金属和可再生生物质衍生碳结合起来以增强 CO 光还原具有良好的前景,这可能会扩展到修饰其他半导体材料以提高活性的更多光催化应用。