分割氢键有机框架的孔道空间提升光催化CO_(2)还原效率  

Partitioning of pore space in hydrogen-bonded organic frameworks for enhanced CO_(2) photoreduction

作　　者：王子祥 邹莹 方志斌 李金林 李亚峰 张安安 刘天赋 Zi-Xiang Wang;Ying Zou;Zhi-Bin Fang;Jin-Lin Li;Yafeng Li;An-An Zhang;Tian-Fu Liu(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)

机构地区：[1]College of Chemistry,Fuzhou University,Fuzhou 350002,China [2]State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China [3]Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou 350002,China

出　　处：《Science China Materials》2024年第6期1846-1850,共5页中国科学（材料科学）（英文版）

基　　金：supported by the National Natural Science Foundation of China (22071246 and 22272178);CAS youth interdisciplinary team (JCTD-2022-12);CAS-Iranian Vice presidency for science and technology joint research project (121835KYSB20200034);China Postdoctoral Science Foundation (2023M733499)。

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CO_(2)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.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 CO_(2) 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…πinterac-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.

关 键 词：hydrogen-bonded organic frameworks CO_(2)photo-reduction pore space partitioning strategy 

分 类 号：X701[环境科学与工程—环境工程] O643.36[理学—物理化学] O644.1[理学—化学]