Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) , Tianjin 300072, China.
ACS Nano. 2017 Jan 24;11(1):1103-1112. doi: 10.1021/acsnano.6b08251. Epub 2017 Jan 3.
Inspired by the orderly stacked nanostructure and highly integrated function of thylakoids in a natural photosynthesis system, multishell g-CN (MSCN) nanocapsule photocatalysts have been prepared by SiO hard template with different shell layers. The resultant triple-shell g-CN (TSCN) nanocapsules display superior photocatalysis performance to single-shell and double-shell counterparts owing to excellent visible-light harvesting and electron transfer properties. Specially, with the increase of the shell layer number, light harvesting is greatly enhanced. There is an increase of the entire visible range absorption arising from the multiple scattering and reflection of the incident light within multishell nanoarchitectures as well as the light transmission within the porous thin shells, and an increase of absorption edge arising from the decreased quantum size effect. The electron transfer is greatly accelerated by the mesopores in the thin shells as nanoconduits and the high specific surface area of TSCN (310.7 m g). With the tailored hierarchical nanostructure features, TSCN exhibits a superior visible-light H-generation activity of 630 μmol h g (λ > 420 nm), which is among one of the most efficient metal-free g-CN photocatalysts. This study demonstrates a bioinspired approach to the rational design of high-performance nanostructured visible-light photocatalysts.
受自然界光合作用系统中类囊体有序堆叠的纳米结构和高度集成功能的启发,我们采用 SiO2 硬模板制备了具有不同壳层数的多壳层 g-CN(MSCN)纳米胶囊光催化剂。由于具有优异的可见光捕获和电子转移性能,所得的三层 g-CN(TSCN)纳米胶囊比单壳和双壳对照物具有更好的光催化性能。特别地,随着壳层数的增加,光捕获得到了极大的增强。多壳纳米结构内入射光的多次散射和反射以及多孔薄壳内的光传输导致整个可见光范围的吸收增加,并且由于量子尺寸效应的减小,吸收边增加。薄壳中的介孔作为纳米通道和 TSCN(310.7 m²/g)的高比表面积极大地加速了电子转移。通过定制的分级纳米结构特征,TSCN 表现出优异的可见光 H2 生成活性(630 μmol h g(λ > 420 nm)),这是最高效的无金属 g-CN 光催化剂之一。本研究展示了一种基于生物启发的方法来合理设计高性能纳米结构可见光光催化剂。