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Binary molecular-semiconductor p–n junctions for photoelectrocatalytic CO2 reduction

Bing Shan, Srinivas Vanka, Ting-Ting Li, Ludovic Troian-Gautier, M. Kyle Brennaman, Zetian Mi and Thomas J. Meyer ()
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Bing Shan: University of North Carolina at Chapel Hill
Srinivas Vanka: University of Michigan
Ting-Ting Li: University of North Carolina at Chapel Hill
Ludovic Troian-Gautier: University of North Carolina at Chapel Hill
M. Kyle Brennaman: University of North Carolina at Chapel Hill
Zetian Mi: University of Michigan
Thomas J. Meyer: University of North Carolina at Chapel Hill

Nature Energy, 2019, vol. 4, issue 4, 290-299

Abstract: Abstract In one approach to solar energy conversion, light-harvesting sensitizers absorb and convert photons into electron–hole pairs to drive water splitting or CO2 reduction to produce fuels. Despite recent progress in photoelectrocatalytic cells, experimental realization of a high-performance photocathode for solar-driven CO2 reduction has proven difficult. Here, we use a binary p–n junction strategy to prepare a series of photocathodes that convert sunlight into high-energy electrons for efficient CO2 reduction to formate. The photocathodes integrate a semiconductor p–n junction comprising GaN nanowire arrays on silicon, with molecular p–n junctions self-assembled on the semiconductor surface. Solar irradiation of the photocathodes generates redox-separated states that interact to form an intermediate state with remotely separated electrons and holes at the catalyst and semiconductor, respectively. The photocathodes reduce CO2 to formate at stable photocurrent densities of around −1.1 mA cm−2 during 20 h of irradiation with Faradaic efficiencies of up to 64%.

Date: 2019
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DOI: 10.1038/s41560-019-0345-y

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