Construction of COF/COF Organic S-Scheme Heterostructure for Enhanced Overall Water Splitting

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Bing-Bing Luan, Xiaoyu Chu, Ya Wang, Xiu Qiao, Yanxia Jiang, Feng-Ming Zhang
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引用次数: 0

Abstract

Covalent organic frameworks (COFs) as a new type of photocatalysts have shown unique advantages in visible-light-driven hydrogen evolution, while the reported overall water-splitting systems are still very rare among various COF-based photocatalysts. Herein, two COFs are integrated to construct a type of organic S-scheme heterojunction for improved overall water splitting. In this system, TpBpy-COF and COF-316 serve as H2- and O2-evolving components, respectively, which are combined through π–π interaction between conjugated aromatic rings. By introducing ultra-small Pt nanoparticles (NPs) into the pores of the TpBpy-COF nanosheets (NS), the resultant COF-316/Pt@TpBpy-COF NS heterostructure achieves extremely high H2 and O2 evolution rates of 220.4 and 110.2 µmol g−1 h−1, respectively, under visible light irradiation (λ ≥ 420 nm). The results of transient absorption spectra (TAS) and photoelectronic measurements indicate that the organic heterojunction interface notably facilitates the separation and transfer of photogenerated electron-hole pairs. Further, theoretical calculations and in situ experiments confirm the spontaneous formation of the COF/COF heterojunction interface and the active sites for overall water splitting.

Abstract Image

构建 COF/COF 有机 S-Scheme 异质结构以提高整体水分离效果
共价有机框架(COFs)作为一种新型光催化剂,在可见光驱动的氢气进化中显示出独特的优势,但在各种基于 COFs 的光催化剂中,整体水分离系统的报道仍然非常罕见。在此,我们将两种 COF 集成在一起,构建了一种有机 S 型异质结,从而提高了整体水分离效果。在该体系中,TpBpy-COF 和 COF-316 分别作为 H2-和 O2-发生组分,通过共轭芳香环之间的 π-π 相互作用结合在一起。通过在 TpBpy-COF 纳米片(NS)的孔隙中引入超小型铂纳米颗粒(NPs),在可见光照射(λ ≥ 420 nm)下,COF-316/Pt@TpBpy-COF NS 异质结构实现了极高的 H2 和 O2 演化率,分别达到 220.4 和 110.2 µmol g-1 h-1。瞬态吸收光谱(TAS)和光电子测量结果表明,有机异质结界面显著促进了光生电子-空穴对的分离和转移。此外,理论计算和现场实验证实了 COF/COF 异质结界面的自发形成以及整体水分离的活性位点。
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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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