Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 16, Pages 5326-5329Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b01601
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Funding
- National Science Foundation [DMR-1308229, NSF/DMR-1531283]
- China Scholarship Council
- Division of Chemistry (CHE), National Science Foundation [NSF/CHE-1346572]
- U.S. DOE [DE-AC02-06CH11357]
- Division of Materials Research (DMR), National Science Foundation [NSF/CHE-1346572]
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We report the design of two new metal organic frameworks (MOFs), Ru-TBP and Ru-TBP-Zn, based on Ru-2 secondary building units (SBUs) and porphyrin-derived tetracarboxylate ligands. The proximity of Ru-2 SBUs to porphyrin ligands (similar to 1.1 nm) facilitates multielectron transfer from excited porphyrins to Ru-2 SBUs to enable efficient visible-light-driven hydrogen evolution reaction (HER) in neutral water. Photophysical and electrochemical studies revealed oxidative quenching of excited porphyrin by Ru-2 SBUs as the initial step of the HER process and the energetics of key intermediates in the catalytic cycle. Our work provides a new strategy to building multifunctional MOFs with synergistic ligands and SBUs for efficient photocatalysis.
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