期刊
ACS CATALYSIS
卷 11, 期 4, 页码 2098-2107出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04820
关键词
covalent organic framework; photosystem I; photocatalysis; water splitting; H-2 evolution
资金
- National Key Research and Development Program of China [2020YFA0907300]
- National Natural Science Foundation of China [21871153, 31800793]
- 111 Project [B12015]
The article discusses the development of a photocatalyst based on covalent organic frameworks for visible-light-driven water splitting to produce hydrogen. Inspired by the structure of photosystem I, the authors designed a framework with high photocatalytic activity.
Developing photocatalysts capable of visible-light-driven water splitting to produce clean hydrogen (H-2) is one of the premier challenges for solar energy conversion into clean and sustainable fuels. Inspired from the structure feature of photosystem I in nature, we have designed and synthesized a series of robust covalent organic frameworks (NKCOFs = Nankai University COFs) based on electric donor-acceptor moieties, in which the electron-donor group of pyrene can be used for harvesting light. Meanwhile, benzothiadiazole with different functional groups was introduced as an electron acceptor to tune the light-adsorption ability of COFs. Notably, the activity of NKCOF-108 for photochemical H-2 evolution under visible light was among the highest in COFs without hybridization with other materials. We attribute the high hydrogen evolution rate of NKCOF-108 to its distinct structural features and wide visible-light-response range. The highly ordered layered structure ensures that sufficient active sites are accessible for H-2 production, and the donor-acceptor design can promote the separation of photogenerated carriers. Our findings have provided an effective strategy to design photocatalysts for light-driven H-2 evolution.
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