Photoexcited radical anion super-reductants for solar fuels catalysis

Journal Article · Sun Apr 01 00:00:00 EDT 2018 · Coordination Chemistry Reviews

DOI:https://doi.org/10.1016/j.ccr.2018.01.018· OSTI ID:1462686

La Porte, Nathan T. ^[1]; Martinez, Jose F. ^[1]; Chaudhuri, Subhajyoti ^[2]; Hedstr�m, Svante ^[3]; Batista, Victor S. ^[2]; Wasielewski, Michael R. ^[1]

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1. Northwestern University, Evanston, IL (United States). Department of Chemistry, Argonne-Northwestern Solar Energy Research Center, and Institute for Sustainability and Energy at Northwestern
2. Yale University, New Haven, CT (United States). Department of Chemistry, Argonne-Northwestern Solar Energy Research Center, and Yale Energy Sciences Institute
3. Stockholm University, Stockholm, (Sweden). Department of Physics, AlbaNova University Center

The catalytic transformation of carbon dioxide into fuels is one of the most important reactions forcreating a sustainable, carbon-neutral energy economy. Given that the sun is the only plausible energysource that can accommodate the increased global energy demand without contributing to catastrophicclimate change, it makes sense to use solar energy to drive this reaction, ideally using the largest possibleportion of the solar spectrum. Over the past several years, we have explored the use of reduced rylenedi-imide chromophores, which absorb wavelengths ranging into the near-infrared, as strongly reducingphotosensitizers capable of photosensitizing Re(diimine)(CO)3L metal centers towards the binding andreduction of CO2. We have explored the effects of varying the binding geometry, donor–acceptor redoxpotentials, and excitation wavelength on the kinetics of electron transfer from the reduced rylenediimideto the metal center. So far, we have achieved charge-separated lifetimes in electrocatalytically activecomplexes of 25 ns when illuminated with near-infrared light, and >250 ns when illuminated with blue light.

• Research Organization: Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
• Sponsoring Organization: USDOE
• DOE Contract Number: SC0001059
• OSTI ID: 1462686
• Journal Information: Coordination Chemistry Reviews, Vol. 361, Issue C; ISSN 0010-8545
• Country of Publication: United States
• Language: English