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用于双相流体系统中连续光催化合成和萃取过氧化氢的全氟烷基改性共价有机框架

Perfluoroalkyl-modified covalent organic frameworks for continuous photocatalytic hydrogen peroxide synthesis and extraction in a biphasic fluid system.

作者信息

Shao Chaochen, Yu Xiaohan, Ji Yujin, Xu Jie, Yan Yuchen, Hu Yongpan, Li Youyong, Huang Wei, Li Yanguang

机构信息

Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 215123, Suzhou, China.

Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, 215123, Suzhou, China.

出版信息

Nat Commun. 2024 Sep 13;15(1):8023. doi: 10.1038/s41467-024-52405-3.

Abstract

HO photosynthesis represents an appealing approach for sustainable and decentralized HO production. Unfortunately, current reactions are mostly carried out in laboratory-scale single-phase batch reactors, which have a limited HO production rate (<100 μmol h) and cannot operate in an uninterrupted manner. Herein, we propose continuous HO photosynthesis and extraction in a biphasic fluid system. A superhydrophobic covalent organic framework photocatalyst with perfluoroalkyl functionalization is rationally designed and prepared via the Schiff-base reaction. When applied in a home-built biphasic fluid photo-reactor, the superhydrophobicity of our photocatalyst allows its selective dispersion in the oil phase, while formed HO is spontaneously extracted to the water phase. Through optimizing reaction parameters, we achieve continuous HO photosynthesis and extraction with an unprecedented production rate of up to 968 μmol h and tunable HO concentrations from 2.2 to 38.1 mM. As-obtained HO solution could satisfactorily meet the general demands of household disinfection and wastewater treatments.

摘要

光催化产过氧化氢是一种实现可持续和分散式过氧化氢生产的有吸引力的方法。不幸的是,目前的反应大多在实验室规模的单相间歇反应器中进行,其过氧化氢产率有限(<100 μmol/h),且无法连续运行。在此,我们提出在双相流体系统中进行连续的光催化产过氧化氢及萃取。通过席夫碱反应合理设计并制备了具有全氟烷基功能化的超疏水共价有机框架光催化剂。当应用于自制的双相流体光反应器时,我们的光催化剂的超疏水性使其能够选择性地分散在油相中,而生成的过氧化氢则自发萃取到水相中。通过优化反应参数,我们实现了连续的光催化产过氧化氢及萃取,产率高达968 μmol/h,这是前所未有的,并且过氧化氢浓度可在2.2至38.1 mM之间调节。所得到的过氧化氢溶液能够令人满意地满足家庭消毒和废水处理的一般需求。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a704/11399338/2d3743a345fe/41467_2024_52405_Fig1_HTML.jpg

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