分割氢键有机框架的孔道空间提升光催化CO2还原效率
Partitioning of pore space in hydrogen-bonded organic frameworks for enhanced CO2 photoreduction
王子祥 1邹莹 1方志斌 2李金林 3李亚峰 4张安安 2刘天赋2
作者信息
- 1. 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
- 2. 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
- 3. State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China
- 4. College of Chemistry,Fuzhou University,Fuzhou 350002,China
- 折叠
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.
Abstract
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.
关键词
hydrogen-bonded organic frameworks/CO2 photo-reduction/pore space partitioning strategyKey words
hydrogen-bonded organic frameworks/CO2 photo-reduction/pore space partitioning strategy引用本文复制引用
基金项目
National Natural Science Foundation of China(22071246)
National Natural Science Foundation of China(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)
出版年
2024
NETL
NSTL
万方数据