Metal-Organic Frameworks Integrate Cu Photosensitizers and Secondary Building Unit-Supported Fe Catalysts for Photocatalytic Hydrogen Evolution

We report here the synthesis of a series of metal-organic frameworks (MOFs), , comprising cuprous photosensitizing linkers (Cu-PSs) and catalytically active Fe centers supported on secondary building units (SBUs) for photocatalytic H evolution. Close proximity (∼1 nm) between Cu-PS and SBU-supported...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2020-06, Vol.142 (23), p.10302-10307
Main Authors: Pi, Yunhong, Feng, Xuanyu, Song, Yang, Xu, Ziwan, Li, Zhong, Lin, Wenbin
Format: Article
Language:English
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Summary:We report here the synthesis of a series of metal-organic frameworks (MOFs), , comprising cuprous photosensitizing linkers (Cu-PSs) and catalytically active Fe centers supported on secondary building units (SBUs) for photocatalytic H evolution. Close proximity (∼1 nm) between Cu-PS and SBU-supported Fe sites and stabilization of Fe sites by periodically ordered SBUs led to exceptionally high H evolution activity for , with turnover numbers of up to 33 700 and turnover frequencies of up to 880 h . Photocatalytic H evolution activities of correlate with the lability of X counteranions, suggesting that open coordination environments of Fe sites generated by labile X groups facilitate the formation of Fe-hydride intermediates before hydrogen evolution. This work highlights the potential of using MOFs to integrate Earth-abundant components for solar energy utilization.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.0c03906