期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 122, 期 5, 页码 2608-2617出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.7b11999
关键词
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资金
- Argonne Northwestern Solar Energy Research (ANSER) Center, an Energy Frontier Research Center - U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0001059]
- Qatar National Research Fund (Qatar Foundation) [9-174-2-092]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205]
- State of Illinois
- International Institute for Nanotechnology (IIN)
Electron donor-acceptor photosensitizers having long charge separation lifetimes and high-reducing potentials that can be easily appended to thermodynamically difficult to reduce catalysts hold great promise for driving CO2 reduction. This study presents a new molecular triad utilizing a naphthalene diimide radical anion (NDI center dot-) donor chromophore appended to a 9,10-diphenylanthracene (DPA) acceptor, which is in turn linked to Re(bpy)(CO)(3)Cl. The NDI center dot- chromophore is readily generated by mild chemical or electrochemical reduction, absorbs at wavelengths as long as 800 nm, and has an excited state oxidation potential (-2.1 V vs SCE), which rivals or exceeds those of metalorganic and organometallic chromophores. Photoexcitation of NDI center dot- to *NDI center dot- is followed by ultrafast reduction of DPA to DPA(center dot-), which then rapidly reduces the metal complex. The overall quantum yield for reduction of Re(bpy)(CO)(3)Cl is approximately 90% using visible light. The overall time constant for the forward electron transfer to reduce the metal complex is tau = 14.5 ps, while the time constant for back-electron transfer is tau = 24.5 ns. Under typical electrocatalytic conditions, the molecular triad demonstrates electrochemical reduction of CO2.
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