Unbiased Sunlight-Driven Artificial Photosynthesis of Carbon Monoxide from CO2 Using a ZnTe-Based Photocathode and a Perovskite Solar Cell in Tandem

Solar fuel production, mimicking natural photosynthesis of converting CO2 into useful fuels and storing solar energy as chemical energy, has received great attention in recent years. Practical large-scale fuel production needs a unique device capable of CO2 reduction using only solar energy and water as an electron source. Here we report such a system composed of a gold-decorated triple-layered ZnO@ZnTe@CdTe core-shell nanorod array photocathode and a CH3NH3PbI3 perovskite solar cell in tandem. The assembly allows effective light harvesting of higher energy photons (>2.14 eV) from the front-side photocathode and lower energy photons (>1.5 eV) from the back-side-positioned perovskite solar cell in a single-photon excitation. This system represents an example of a photocathode-photovoltaic tandem device operating under sunlight without external bias for selective CO2 conversion. It exhibited a steady solar-to-CO conversion efficiency over 0.35% and a solar-to-fuel conversion efficiency exceeding 0.43% including H-2 as a minor product.