共价有机骨架和光敏金属有机环的杂化：构建超分子Z型异质结构用于超高光催化析氢的新策略,Aggregate

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共价有机骨架和光敏金属有机环的杂化：构建超分子Z型异质结构用于超高光催化析氢的新策略
Aggregate ( IF 13.9 ) Pub Date : 2023-10-10 , DOI: 10.1002/agt2.442
Xin‐Ao Li ₁ , Zi‐Zhan Liang ₁ , Ye‐Cheng Zhou ₁ , Jian‐Feng Huang ₁ , Xiao‐Lin Wang ₁ , Li‐Min Xiao ₂ , Jun‐Min Liu ₁

Affiliation

基于共价有机框架（COF）的Z型异质结光系统的合理设计是利用太阳能进行氢转化的一种有前途的策略。在此，通过珊瑚状COF（S-COF）和光敏Pd ₂ L ₂型金属有机环（MAC-）的超分子相互作用，构建了基于COF和金属有机环的直接Z型单原子光催化剂。FA1）。 MAC-FA1/S-COF异质结表现出良好的光吸收、高效的电荷分离和转移、缓慢的电子-空穴复合以及高度分散的Pd活性位点，从而实现高效稳定的H ₂析出反应。优化后的4% MAC-FA1/S-COF在5小时内实现100 mmol g ^-1 h ^-1的H₂析出速率，并在20小时内获得相对于Pd的总累积周转数（TON _Pd）437,685 ，远优于S-COF、MAC-FA1、M-5/S-COF、Pd/S-COF和M-5/Pd/S-COF，是COF基光催化剂中最高记录之一太阳能驱动的H ₂演化。这是第一个将光敏金属有机环/笼纳入多孔晶体COF中形成超分子Z型异质结的工作，该异质结作为太阳能驱动H ₂生产的高性能光催化剂具有巨大潜力。

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Hybridization of covalent organic frameworks and photosensitive metal-organic rings: A new strategy for constructing supramolecular Z-scheme heterostructures for ultrahigh photocatalytic hydrogen evolution

The rational design of Z-scheme heterojunction photosystems based on covalent organic frameworks (COFs) is a promising strategy for harnessing solar energy for hydrogen conversion. Herein, a direct Z-scheme single-atom photocatalyst based on COF and metal-organic ring has been constructed through the supramolecular interactions of coral-like COF (S-COF) and photosensitized Pd₂L₂ type metal-organic ring (MAC-FA1). The MAC-FA1/S-COF heterojunction exhibits good light absorption, efficient charge separation and transfer, slow electron-hole recombination, and highly dispersed Pd active sites, enabling an efficient and stable H₂ evolution reaction. The optimized 4% MAC-FA1/S-COF achieves an H₂ evolution rate of 100 mmol g⁻¹ h⁻¹ within 5 h and obtains a total accumulated turn-over number relative to Pd (TON_Pd) of 437,685 within 20 h, far superior to S-COF, MAC-FA1, M-5/S-COF, Pd/S-COF, and M-5/Pd/S-COF, which is one of the highest records among COF-based photocatalysts for solar-driven H₂ evolution. This is the first work to incorporate photosensitized metal-organic rings/cages into porous crystalline COFs to form a supramolecular Z-scheme heterojunction, which has significant potential as a high-performance photocatalyst for solar-driven H₂ production.

更新日期：2023-10-10

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