Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 38, Pages 14961-14965Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b07067
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Funding
- U.S. Air Force Office of Scientific Research (AFOSR), Basic Research Initiative (BRI) [FA9550-12-1-0414]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0016450]
- U.S. Department of Energy (DOE) [DE-SC0016450] Funding Source: U.S. Department of Energy (DOE)
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We report the enhancement of photocatalytic performance by introduction of hydrogen-bonding interactions to a Re bipyridine catalyst and Ru photosensitizer system (ReDAC/RuDAC) by the addition of amide substituents, with carbon monoxide (CO) and carbonate/bicarbonate as products. This system demonstrates a more-than-3-fold increase in turnover number (TONCO = 100 +/- 4) and quantum yield (Phi(CO) = 23.3 +/- 0.8%) for CO formation compared to the control system using unsubstituted Ru photosensitizer (RuBPY) and ReDAC (TONCO = 28 +/- 4 and Phi(CO) = 7 +/- 1%) in acetonitrile (MeCN) with 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH) as sacrificial reductant. In dimethylformamide (DMF), a solvent that disrupts hydrogen bonds, the ReDAC/RuDAC system showed a decrease in catalytic performance while the control system exhibited an increase, indicating the role of hydrogen bonding in enhancing the photocatalysis for CO2 reduction through supramolecular assembly. The similar properties of RuDAC and RuBPY demonstrated in lifetime measurements, spectroscopic analysis, and electrochemical and spectroelectrochemical studies revealed that the enhancement in photocatalysis is due not to differences in intrinsic properties of the catalyst or photosensitizer, but to hydrogen-bonding interactions between them.
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