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The most efficient catalysts for solar fuel production should operate close to reversible potentials, yet possess a bias for the fuel-forming direction. Protein film electrochemical studies of Ni-containing carbon monoxide dehydrogenase and [NiFeSe]-hydrogenase, each a reversible electrocatalyst, show that the electronic state of the electrode strongly biases the direction of electrocatalysis of CO2/CO and H(+)/H2 interconversions. Attached to graphite electrodes, these enzymes show high activities for both oxidation and reduction, but there is a marked shift in bias, in favor of CO2 or H(+) reduction, when the respective enzymes are attached instead to n-type semiconductor electrodes constructed from CdS and TiO2 nanoparticles. This catalytic rectification effect can arise for a reversible electrocatalyst attached to a semiconductor electrode if the electrode transforms between semiconductor- and metallic-like behavior across the same narrow potential range (&lt;0.25 V) that the electrocatalytic current switches between oxidation and reduction.

journal of the american chemical society

How Light-Harvesting Semiconductors Can Alter the Bias of Reversible Electrocatalysts in Favor of H<sub>2</sub> Production and CO<sub>2</sub> Reduction

How Light-Harvesting Semiconductors Can Alter the Bias of Reversible Electrocatalysts in Favor of H2 Production and CO2 Reduction

How Light-Harvesting Semiconductors Can Alter the Bias of Reversible Electrocatalysts in Favor of H₂ Production and CO₂ Reduction