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通过构建共价异质结来提高 UIO-66-NH/共价三嗪基框架复合材料的光催化 H2 析出性能。

Boosting photocatalytic H evolution on UIO-66-NH/covalent triazine-based frameworks composites by constructing a covalent heterojunction.

机构信息

Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province, College of Environment, Zhejiang University of Technology, Hangzhou, 310032, China.

Ningbo Key Laboratory of Agricultural Germplasm Resources Mining and Environmental Regulation, College of Science and Technology, Ningbo University, Ningbo, 315300, China.

出版信息

Environ Sci Pollut Res Int. 2023 Nov;30(51):111039-111050. doi: 10.1007/s11356-023-30258-5. Epub 2023 Oct 6.

Abstract

Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have been proved as efficient catalysts for photocatalytic hydrogen (H) evolution, thanks to their tunable functionalities, permanent porosity, excellent visible light response, and physicochemical stability. Herein, a series of photocatalysts (termed NUBC) was fabricated by loading different amounts of Zr-UiO-66-NH (NU) onto a benzoic acid-modified covalent triazine-based framework (BC) based on post-synthetic covalent modification. The resulting NUBC catalysts exhibited a type-II Z-scheme heterojunction structure formed via the amide covalent bonds between the amine groups on NU and carboxyl groups on BC. The optimal loading of NU on BC is 30 wt.% (30NUBC) and the corresponding photocatalytic H evolution rate was 378 μmol h g, almost 445 and 2 times than that of NU and BC, respectively. The synergistic effect between the type-II Z-scheme heterojunctions and amide bonds was conducive to boosting visible light harvesting and facilitating charge transportation and separation. Furthermore, the prepared NUBC catalysts show great reusability and stability. Overall, this work sheds light on the design of novel MOF/COF hybrid materials and provides a systematic exploration of their photocatalytic H evolution properties.

摘要

金属-有机骨架(MOFs)和共价有机骨架(COFs)已被证明是高效的光催化析氢(H)催化剂,这要归功于它们可调的功能、永久的多孔性、出色的可见光响应和物理化学稳定性。在此,通过后合成共价修饰,将不同量的 Zr-UiO-66-NH(NU)负载到苯甲酸改性的基于共价三嗪的骨架(BC)上,制备了一系列光催化剂(称为 NUBC)。所得的 NUBC 催化剂表现出通过 NU 上的胺基和 BC 上的羧基之间的酰胺共价键形成的 II 型 Z 型异质结结构。BC 上 NU 的最佳负载量为 30wt.%(30NUBC),相应的光催化 H 析出速率为 378 μmol h g,分别是 NU 和 BC 的 445 倍和 2 倍。II 型 Z 型异质结和酰胺键之间的协同效应有利于提高可见光的捕获,并促进电荷的传输和分离。此外,所制备的 NUBC 催化剂具有很好的可重复使用性和稳定性。总的来说,这项工作为设计新型 MOF/COF 杂化材料提供了思路,并对其光催化 H 析出性能进行了系统的探索。

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