Abstract
There is a global effort to convert sunlight into fuels by photoelectrochemically splitting water to form hydrogen fuels, but the dioxygen byproduct bears little economic value. This raises the important question of whether higher value commodities can be produced instead of dioxygen. We report here photoelectrochemistry at a BiVO4 photoanode involving the oxidation of substrates in organic media. The use of MeCN instead of water enables a broader set of chemical transformations to be performed (e.g., alcohol oxidation and C-H activation/oxidation), while suppressing photocorrosion of BiVO4 that otherwise occurs readily in water, and sunlight reduces the electrical energy required to drive organic transformations by 60%. These collective results demonstrate the utility of using photoelectrochemical cells to mediate organic transformations that otherwise require expensive and toxic reagents or catalysts.
Highlights
There is a global effort to convert sunlight into fuels by photoelectrochemically splitting water to form hydrogen fuels, but the dioxygen byproduct bears little economic value
While there has been a large global effort to reduce the relatively large energy losses associated with producing oxygen at the anode, strikingly few photoanodes are known to be capable of both absorbing incident sunlight and mediating efficient and sustained water oxidation catalysis[7,8,9,10,11]
The BiVO4 photoanodes used in this study were synthesized in accordance with documented procedures[28]
Summary
There is a global effort to convert sunlight into fuels by photoelectrochemically splitting water to form hydrogen fuels, but the dioxygen byproduct bears little economic value. We report here the use of a PEC cell to mediate organic oxidation reactions using a photoanode immersed in organic media. The photoelectrochemical oxidation of benzyl alcohol, cyclohexene, and tetralin into their corresponding carbonyl compounds were demonstrated in a PEC cell containing a BiVO4 photoanode immersed in MeCN containing appropriate reaction mediators (e.g., electrolyte, base, and electron transfer reagent).
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