Single-Atom Metal Sites Anchored Hydrogen-Bonded Organic Frameworks for Superior 'Two-In-One' Photocatalytic Reaction

Shiyu Huang; Yuan Chang; Zhuwei LiJiaqi CaoYurou SongJunfeng GaoLicheng SunJungang Hou

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Single-Atom Metal Sites Anchored Hydrogen-Bonded Organic Frameworks for Superior 'Two-In-One' Photocatalytic Reaction

机译：Single-Atom Metal Sites Anchored Hydrogen-Bonded Organic Frameworks for Superior 'Two-In-One' Photocatalytic Reaction

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Photoredox catalysis is a green solution for organics transformation and CO_2 conversion into valuable fuels, meeting the challenges of sustainable energy and environmental concerns. However, the regulation of singleatomic active sites in organic framework not only influences the photoredox performance, but also limits the understanding of the relationship for photocatalytic selective organic conversion with CO_2 valorization into one reaction system. As a prototype, different single-atomic metal (M) sites (M~(2+) = Fe~(2+), Co~(2+), Ni~(2+), Cu~(2+), and Zn~(2+)) in hydrogen-bonded organic frameworks (M-HOF) backbone with bridging structure of metalnitrogen are constructed by a typical “two-in-one” strategy for superior photocatalytic C-N coupling reactions integrated with CO_2 valorization. Remarkably, Zn-HOF achieves 100% conversion of benzylamine oxidative coupling reactions, 91% selectivity of N-benzylidenebenzylamine and CO_2 conversion in one photoredox cycle. From X-ray absorption fine structure analysis and density functional theory calculations, the superior photocatalytic performance is attributed to synergic effect of atomically dispersed metal sites and HOF host, decreasing the reaction energy barriers, enhancing CO_2 adsorption and forming benzylcarbamic acid intermediate to promote the redox recycle. This work not only affords the rational design strategy of single-atom active sites in functional HOF, but also facilitates the fundamental insights upon the mechanism of versatile photoredox coupling reaction systems.

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《Advanced functional materials》 |2023年第21期|2211631.1-2211631.12|共12页
作者
Shiyu Huang; Yuan Chang; Zhuwei LiJiaqi CaoYurou SongJunfeng GaoLicheng SunJungang Hou;
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Laboratory of Materials Modification by Laser Ion and Electron Beams, Ministry of Education Dalian University of Technology Dalian 116024, P. R. China;

Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry School of Science Westlake University Hangzhou 310024, P. R. China,School of Engineering Sciences in Chemistry Biotechnology and Health KTH Royal Institute of Technology Stock;

State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Oriented Chemical Engineering School of Chemical Engineering Dalian University of Technology Dalian 116024, P. R. China;

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CO_2 valorization; hydrogen-bonded organic frameworks; photocatalytic coupling reactions; photoredox catalysis; single-atomic active sites;

Single-Atom Metal Sites Anchored Hydrogen-Bonded Organic Frameworks for Superior 'Two-In-One' Photocatalytic Reaction

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