Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 23, Pages 10302-10307Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c03906
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Funding
- NSF [CHE-1464941]
- University of Chicago
- Materials Research Collaborative Access Team (MRCAT)
- U.S. DOE [DE-AC02-06CH11357]
- China Scholarship Council
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We report here the synthesis of a series of metal-organic frameworks (MOFs), FeX@Zr-6-Cu, comprising cuprous photosensitizing linkers (Cu-PSs) and catalytically active Fe-II centers supported on secondary building units (SBUs) for photocatalytic H-2 evolution. Close proximity (similar to 1 nm) between Cu-PS and SBU-supported Fe sites and stabilization of Fe sites by periodically ordered SBUs led to exceptionally high H-2 evolution activity for FeX@Zr-6-Cu, with turnover numbers of up to 33 700 and turnover frequencies of up to 880 h(-1). Photocatalytic H-2 evolution activities of FeX@Zr-6-Cu 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.
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