BioChem - DOS

Light-Driven H2 Evolution and C=C or C=O Bond Hydrogenation by Shewanella oneidensis: A Versatile Strategy for Photocatalysis by Nonphotosynthetic Microorganisms

ACS catalysis

Rowe, Sam F.; Le Gall, Gwé naë lle; Ainsworth, Emma V.; Davies, Jonathan A.; Lockwood, Colin W. J.; Shi, Liang; Elliston, Adam; Roberts, Ian N.; Waldron, Keith W.; Richardson, David J.; Clarke, Thomas A.; Jeuken, Lars J. C.; Reisner, Erwin; Butt, Julea N.

<P>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<SUB>2</SUB> evolution or the hydrogenation of C&#xe5fb;C and C&#xe5fb;O bonds in a nonphotosynthetic microorganism. Methylviologen shuttles photoenergized electrons from water-soluble photosensitizers to enzymes that catalyze H<SUB>2</SUB> evolution and the reduction of fumarate, pyruvate, and CO<SUB>2</SUB> in <I>Shewanella oneidensis</I>. 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.</P><BR>[FIG OMISSION]</BR>

2017

American Chemical Society

2155-5435

7

11

pp.7558-7566

10.1021/acscatal.7b02736

http://click.ndsl.kr/servlet/OpenAPIDetailView?keyValue=05787966&target=NART&cn=NART78936740

proton reduction; CO2 reduction; photocatalysis; hydrogenase; formate dehydrogenase; visible light