Journal
ACS CATALYSIS
Volume 7, Issue 11, Pages 7558-7566Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b02736
Keywords
proton reduction; CO2 reduction; photocatalysis; hydrogenase; formate dehydrogenase; visible light
Categories
Funding
- U.K. Biotechnology and Biological Sciences Research Council [BB/K009753/1, BB/K010220/1, BB/K009885/1]
- U.K. Biotechnology and Biological Sciences Research Council (Doctoral Training Partnership Ph.D. studentship)
- U.K. Biotechnology and Biological Sciences Research Council (iCASE Ph.D. studentship)
- Engineering and Physical Sciences Research Council [EP/M001989/1, 1307196]
- Royal Society Leverhulme Trust Senior Research Fellowship
- Biotechnology and Biological Sciences Research Council [BBS/E/F/00044440, BB/K009753/1, 1368995, BBS/E/F/00044476, BB/K009885/1, 1369608, BB/K010220/1] Funding Source: researchfish
- Engineering and Physical Sciences Research Council [1307196, EP/M001989/1] Funding Source: researchfish
- BBSRC [BBS/E/F/00044440, BB/K009885/1, BB/K010220/1, BBS/E/F/00044476, BB/K009753/1] Funding Source: UKRI
- EPSRC [EP/M001989/1] Funding Source: UKRI
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Photocatalytic chemical synthesis by coupling abiotic photosensitizers to purified enzymes provides an effective way to overcome the low conversion efficiencies of natural photosynthesis while exploiting the high catalytic rates and selectivity of enzymes as renewable, earth-abundant electrocatalysts. However, the selective synthesis of multiple products requires more versatile approaches and should avoid the time-consuming and costly processes of enzyme purification. Here we demonstrate a cell-based strategy supporting light-driven H-2 evolution or the hydrogenation of C=C and C=O bonds in a nonphotosynthetic microorganism. Methylviologen shuttles photoenergized electrons from water-soluble photosensitizers to enzymes that catalyze H-2 evolution and the reduction of fumarate, pyruvate, and CO2 in Shewanella oneidensis. The predominant reaction is selected by the experimental conditions, and the results allow rational development of cell-based strategies to harness nature's intrinsic catalytic diversity for selective light driven synthesis of a wide range of products.
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