Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 4, Issue 2, Pages 608-613Publisher
AMER CHEMICAL SOC
DOI: 10.1021/am2018095
Keywords
water oxidation; electrocatalysis; diazonium grafting; carbon electrode; water splitting
Funding
- UNC EFRC: Solar Fuels, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- UNC
- NSF
- UNC Department of Chemistry
- DOE EPSCoR [DE-FG02-07ER46375]
- DARPA [W911NF-09-1-0267]
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Hydrogen,production from water splitting provides a; potential solution to storing harvested solar energy in chemical fuels,, but this process requires active and robust catalysts that can oxidize water to provide a source of electrons for proton reduction. Here we report the direct, covalent grafting of molecular Ir complexes onto carbon electrodes, with up to a monolayer coverage. Carbon-grafted Ir complexes electrochemically oxidize water with a turnover frequency of up to 3.3 s(-1) and a turnover number of 644 during the first hour. Electrochemical water oxidation with grafted catalysts gave enhanced rates and stability compared to chemically driven water oxidation with the corresponding molecular catalysts. This strategy provides away to systematically evaluate catalysts under tunable conditions, potentially providing new insights into electrochemical water oxidation processes and water oxidation catalyst design.
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