Boosting photocatalytic hydrogen evolution enabled by SiO2-supporting chiral covalent organic frameworks with parallel stacking sequence

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-09-01 DOI:10.1016/S1872-2067(24)60107-5
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Abstract

Two-dimensional covalent organic frameworks (2D COFs) feature extended π-conjugation and ordered stacking sequence, showing great promise for high-performance photocatalysis. Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer, but the precise ordered alignment is limited due to the non-covalent π-stacking of COF layers, accordingly hindering out-of-plane transfer kinetics. Herein, we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO2 microsphere. Compared to the achiral COF analogues, the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration, thereby affording superior photocatalytic performance in hydrogen evolution from water splitting. Taking the simplest ketoenamine-linked chiral COF as a shell of SiO2 particle, the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g–1 h–1 along with the apparent quantum efficiency of 14.31% at 475 nm. Furthermore, the composite photocatalysts could be fabricated into a film device, displaying a remarkable photocatalytic performance of 178.0 mmol m–2 h–1 for hydrogen evolution. Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties.

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利用具有平行堆叠序列的二氧化硅支撑手性共价有机框架促进光催化氢气进化
二维共价有机框架(2D COFs)具有扩展的π共轭和有序堆叠序列,在高性能光催化方面大有可为。二维 COF 的周期性原子框架有利于平面内的光生电荷转移,但由于 COF 层的非共价 π 堆积,其精确有序排列受到限制,从而阻碍了平面外的电荷转移动力学。在此,我们采用手性诱导的方法,在二氧化硅微球的支持下构建了平行叠加堆叠的手性 COF 超薄壳。与非手性 COF 类似物相比,具有平行 AA 叠层结构的手性 COF 壳更有利于增强内置电场,聚集光生电子并使其快速迁移,从而在分水制氢的光催化过程中具有更优越的性能。以最简单的酮胺连接手性 COF 作为 SiO2 粒子的外壳,所得到的复合材料在 475 纳米波长下的氢气进化率达到了惊人的 107.1 mmol g-1 h-1,表观量子效率为 14.31%。此外,这种复合光催化剂还可以制成薄膜装置,在氢气进化方面显示出 178.0 mmol m-2 h-1 的显著光催化性能。我们的工作为有机光催化剂的表面工程提供了支持,并说明了 COF 堆叠结构在调节电子特性方面的重要意义。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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