Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks

IF 18.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

ACS Energy Letters Pub Date : 2024-11-11 DOI:10.1021/acsenergylett.4c0284710.1021/acsenergylett.4c02847

Qing Niu, Wenfeng Deng, Yanlei Chen, Qingqing Lin, Liuyi Li*, Zheyuan Liu, Jinhong Bi* and Yan Yu*,

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引用次数: 0

Abstract

Covalent organic frameworks (COFs) are promising semiconductor photocatalysts but are still limited in overall water splitting mainly owing to a lack of clear design approaches with which to ameliorate catalytic activities. Here, we demonstrate a synergy of exciton dipole orientation and dynamic reactivity of COFs that enables water splitting for stoichiometric evolution of H₂ and O₂. The exciton dipole orientation is responsible for driving the spatial separation of photoinduced charges, while the dynamic reactivity of imine bonds of COFs with water and holes is proven for initiating water oxidation. Accordingly, a rationally designed BtS-COF with benzotrithiophene and sulfone units exhibits a much-improved performance in H₂ and O₂ evolution in neutral water under visible light. Its catalytic efficiency is even superior to some photocatalysts with metal-based water oxidation cocatalyst.

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激子偶极取向和动态反应性协同使共价有机框架中的整体水分裂成为可能

共价有机框架（COFs）是一种很有前途的半导体光催化剂，但由于缺乏明确的设计方法来改善催化活性，其在整体水分解方面仍然受到限制。在这里，我们证明了激子偶极子取向和COFs的动态反应性的协同作用，使H2和O2的化学计量进化中的水分裂成为可能。激子偶极取向驱动了光诱导电荷的空间分离，而COFs的亚胺键与水和空穴的动态反应性被证明是引发水氧化的原因。因此，合理设计的含有苯并三噻吩和砜单元的BtS-COF在可见光下在中性水中的H2和O2析出性能得到了很大改善。其催化效率甚至优于某些具有金属基水氧化助催化剂的光催化剂。

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来源期刊

ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment

CiteScore

31.20

自引率

5.00%

发文量

469

审稿时长

1 months

期刊介绍： ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.