Solar-driven production of hydrogen and acetaldehyde from ethanol on Ni-Cu bimetallic catalysts with solar-to-fuels conversion efficiency up to 3.8

[Display omitted] •An efficient solar-driven ethanol dehydrogenation process is presented.•Remarkable H2 generation rate is achieved over Ni-Cu catalyst by focused solar light.•Solar-to-fuel conversion efficiency up to 3.8 % is reached.•Both photothermal heating and hot carrier generation take responsibility for the high activity. Catalytic ethanol dehydrogenation is recognized as a promising approach to produce valuable chemical stocks, yet its industrialization suffers from high energy consumption. Here, we present an efficient solar-driven ethanol dehydrogenation process using a low-cost Ni-Cu bimetallic catalyst for the high-yield and selective production of H2 and acetaldehyde. Under the irradiation of focused simulated solar light, 176.6 mmol gcatalyst−1 h−1 of H2 production rate with a high solar-to-fuel conversion efficiency (3.8 %) was achieved without additional thermal energy input, which is far more efficient than any previously reported photocatalytic ethanol dehydrogenation systems. Mechanistic investigations revealed that photothermal heating and hot carrier generation over Ni-Cu catalysts took responsibilities for the high activity. Hot electrons generated from Cu nanoparticles could migrate to Ni atoms, which simultaneously favored the separation of charge carriers and the activation of adsorbates. This study opens a promising pathway toward solar-energy conversion technology and advanced cost-effective industrial processes.