Bias-free solar syngas production by integrating a molecular cobalt catalyst with perovskite-BiVO4 tandems.

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The photoelectrochemical (PEC) production of syngas from water and CO2 represents an attractive technology towards a circular carbon economy. However, the high overpotential, low selectivity and cost of commonly employed catalysts pose challenges for this sustainable energy-conversion process. Here we demonstrate highly tunable PEC syngas production by integrating a cobalt porphyrin catalyst immobilized on carbon nanotubes with triple-cation mixed halide perovskite and BiVO4 photoabsorbers. Empirical data analysis is used to clarify the optimal electrode selectivity at low catalyst loadings. The perovskite photocathodes maintain selective aqueous CO2 reduction for one day at light intensities as low as 0.1 sun, which provides pathways to maximize daylight utilization by operating even under low solar irradiance. Under 1 sun irradiation, the perovskite-BiVO4 PEC tandems sustain bias-free syngas production coupled to water oxidation for three days. The devices present solar-to-H2 and solar-to-CO conversion efficiencies of 0.06 and 0.02%, respectively, and are able to operate as standalone artificial leaves in neutral pH solution.

3403 Macromolecular and Materials Chemistry, 34 Chemical Sciences, 3406 Physical Chemistry, 40 Engineering, 4016 Materials Engineering, 7 Affordable and Clean Energy, 12 Responsible Consumption and Production
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Nat Mater
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Springer Science and Business Media LLC
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Biotechnology and Biological Sciences Research Council (BB/K010220/1)
Christian Doppler Forschungsgesellschaft (unknown)
European Research Council (682833)
Christian Doppler Research Association (Austrian Federal Ministry for Digital and Economic Affairs and the National Foundation for Research, Technology and Development), the OMV Group, Cambridge Trusts (Vice-Chancellor’s Award), the Winton Programme for the Physics of Sustainability, BBSRC