Porous Ru-loaded covalent organic framework nanofluids for fast and scalable continuous-flow photocatalytic oxidations

IF 48.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Chao Jiang, Yuhan Wang, Guan Sheng, Yan Liu, Xing Han, Zhongkui Li, Cheng Cheng, Xiangxiang Zhao, Yujie Zhou, Qun Zhang, Minjing Shang, Yihan Zhu, Yuanhai Su, Yong Cui
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引用次数: 0

Abstract

Continuous-flow photocatalysis with heterogeneous catalysts offers a sustainable route for chemical synthesis, but it is limited by catalyst deactivation and inefficient light utilization arising from swelling and pore clogging. Here we develop a high-performance continuous-flow system based on covalent organic framework (COF) nanofluids as porous catalytic dispersions. Two ionic COFs incorporating imine-linked Ru(II)–triphenanthroline photocatalysts are synthesized, featuring triple-helix porous architectures resolved by cryogenic low-dose electron microscopy. Processed into nanofluids with an average particle size below 100 nm, the COFs remain colloidally stable for over seven days without surfactants, enabling efficient mass transfer, light penetration and heat dissipation in flow microreactors. These attributes result in markedly enhanced photocatalytic performance across a range of achiral and chiral oxidation reactions. Notably, artemisinin is produced in 64% yield within 7 min via photooxidation of dihydroartemisinic acid. Integration of a dual-capillary microreactor further doubles productivity, highlighting the scalability and industrial potential of porous nanofluid photocatalysis. Heterogeneous and homogeneous photocatalysts offer different strengths and weaknesses. Here, continuous-flow photocatalytic oxidation reactions are performed using covalent organic framework nanofluids that heterogenize molecular units to combine the advantages of catalyst efficiency, light utilization and easy separation.

Abstract Image

Abstract Image

用于快速和可扩展的连续流光催化氧化的多孔钌负载共价有机框架纳米流体
多相催化剂的连续流光催化为化学合成提供了一条可持续的途径,但受到催化剂失活以及膨胀和孔堵塞引起的光利用率低下的限制。在此,我们开发了一种基于共价有机骨架(COF)纳米流体作为多孔催化分散体的高性能连续流系统。合成了两个含有亚胺连接Ru(II) -三菲罗啉光催化剂的离子COFs,具有三螺旋多孔结构,通过低温低剂量电子显微镜分析。将COFs加工成平均粒径小于100 nm的纳米流体后,在不使用表面活性剂的情况下,其胶体稳定性可保持7天以上,从而在流动微反应器中实现高效的传质、透光和散热。这些特性导致在一系列非手性和手性氧化反应中显著增强光催化性能。值得注意的是,通过双氢青蒿酸的光氧化,在7分钟内以64%的产率生产青蒿素。双毛细管微反应器的集成进一步提高了生产效率,突出了多孔纳米流体光催化的可扩展性和工业潜力。
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来源期刊
Nature Catalysis
Nature Catalysis Chemical Engineering-Bioengineering
CiteScore
52.10
自引率
1.10%
发文量
140
期刊介绍: Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.
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