分割氢键有机框架的孔道空间提升光催化CO2还原效率

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中文摘要：氢键有机框架材料(HOFs)在催化领域具有巨大的潜力,但其孔道空间在去除溶剂后易塌陷,限制了其在光催化能源转换和存储方面的应用.本研究采用孔道分割策略成功设计并合成了一种稳定孔道结构、高效光催化CO2还原活性的HOF催化剂.H4TBAPy分子通过与HOF孔道中大量的CH…π相互作用锚定自身,并将HOF的大孔道分隔成多个小空间,显著增加了HOF框架的稳定性.同时,富电子属性的H4TBAPy分子提升了HOF体系中电子的传输速率,从而提高了催化活性.这项研究为设计稳定、高性能的HOFs光催化剂提供了新策略.

外文标题：Partitioning of pore space in hydrogen-bonded organic frameworks for enhanced CO2 photoreduction

外文摘要：Hydrogen-bonded organic frameworks(HOFs)hold significant promise for catalytic applications.However,the collapse of pores upon solvent removal significantly re-stricts the utility of HOFs in photocatalytic processes for en-ergy production and storage.This work describes HOF-based catalysis with a stable pore structure and efficient catalytic activity that has been designed and tested for CO2 photo-reduction in pure water.In this system,based on HOFs,the 1,3,6,8-tetra(4-carboxyphenyl)pyrene(H4TBAPy)molecules segment the large pore spaces into multiple domains.These molecules,anchored to the HOF via strong CH…π interac-tions,act as rigid auxiliary linkers,notably improving the structural stability within the HOF.Additionally,the in-corporation of electron-rich H4TBAPy molecules expedited electron transport within the HOF,markedly enhancing its catalytic activity.This work provides a new strategy for de-signing stable and high-performance HOF photocatalysts.

外文关键词：

hydrogen-bonded organic frameworksCO2 photo-reductionpore space partitioning strategy

作者：

王子祥、邹莹、方志斌、李金林、李亚峰、张安安、刘天赋

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作者单位：

College of Chemistry,Fuzhou University,Fuzhou 350002,China

State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China

Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou 350002,China

关键词：

hydrogen-bonded organic frameworks CO2 photo-reduction pore space partitioning strategy

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaCAS youth interdisciplinary teamCAS-Iranian Vice presidency for science and technology joint research projectChina Postdoctoral Science Foundation

项目编号：

2207124622272178JCTD-2022-12121835KYSB202000342023M733499

出版年：

2024

DOI：

10.1007/s40843-023-2834-1

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(6)