Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 51, Pages 17830-17834Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b09740
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Funding
- China Scholarship Council [201507040033]
- National Institutes of Health (NIH)'s F32 postdoctoral fellowship [F32GM122392]
- Colorado State University
- National Institute of General Medical Sciences of the NIH [R35GM119702]
- Institut Universitaire de France (IUF)
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Using a phenoxazine-based organic photo-sensitizer and an iron porphyrin molecular catalyst, we demonstrated photochemical reduction of CO2 to CO and CH4 with turnover numbers (TONs) of 149 and 29, respectively, under visible-light irradiation (lambda > 435 nm) with a tertiary amine as sacrificial electron donor. This work is the first example of a molecular system using an earth-abundant metal catalyst and an organic dye to effect complete 8e(-)/8H(+) reduction of CO2 to CH4, as opposed to typical 2e(-)/2H(+) products of CO or formic acid. The catalytic system continuously produced methane even after prolonged irradiation up to 4 days. Using CO as the feedstock, the same reactive system was able to produce CH4 with 85% selectivity, 80 TON and a quantum yield of 0.47%. The redox properties of the organic photo-sensitizer and acidity of the proton source were shown to play a key role in driving the 8e(-)/8H(+) processes.
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