Abstract
Redox enzymes catalyze fascinating chemical reactions with excellent regio- and stereo-specificity. Nicotinamide adenine dinucleotide cofactor is essential in numerous redox biocatalytic reactions and needs to be regenerated because it is consumed as an equivalent during the enzymatic turnover. Here we report on unbiased photoelectrochemical tandem assembly of a photoanode (FeOOH/BiVO4) and a perovskite photovoltaic to provide sufficient potential for cofactor-dependent biocatalytic reactions. We obtain a high faradaic efficiency of 96.2% and an initial conversion rate of 2.4 mM h−1 without an external applied bias for the photoelectrochemical enzymatic conversion of α-ketoglutarate to l-glutamate via l-glutamate dehydrogenase. In addition, we achieve a total turnover number and a turnover frequency of the enzyme of 108,800 and 6200 h−1, respectively, demonstrating that the tandem configuration facilitates redox biocatalysis using light as the only energy source.
Highlights
Redox enzymes catalyze fascinating chemical reactions with excellent regio- and stereospecificity
We report unbiased solar NAD(P)H regeneration and redox biocatalysis using a large-scale, tandem PEC configuration consisting of a nanostructured FeOOH/BiVO4 photoanode, an organometallic perovskite-based photovoltaic cell, and a carbon nanotube (CNT) film cathode
The perovskite solar cell with a light absorber containing triple cations, Cs, formamidinium, and methylammonium absorbs the transmitted light through the FeOOH/BiVO4 photoanode, providing additional photovoltage to satisfy the thermodynamic requirement for both water oxidation and the regeneration of NADH cofactors
Summary
Redox enzymes catalyze fascinating chemical reactions with excellent regio- and stereospecificity. We report unbiased solar NAD(P)H regeneration and redox biocatalysis using a large-scale, tandem PEC configuration consisting of a nanostructured FeOOH/BiVO4 photoanode, an organometallic perovskite-based photovoltaic cell, and a carbon nanotube (CNT) film cathode. To eliminate the need for external bias to drive the target PEC reaction, we used a triple-cation organometallic perovskite solar cell[17] as an additional power source to couple with the FeOOH/BiVO4 photoanode.
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