Abstract
CO(2) conversion to CH(3)OH under mild conditions is of particular interest yet rather challenging. Both electro- and thermo-catalytic CO(2) reduction to CH(3)OH can only produce CH(3)OH in low concentration (typically mixed with water), requiring energy-intensive purification processes. Here we design a sun-simulated-driven tandem catalytic system comprising CO(2) electroreduction to syngas, and further photothermal conversion into high-purity CH(3)OH (volume fraction > 97%). We construct a self-supporting electrocatalyst featuring dual active sites of Ni single atoms and encapsulated Co nanoparticles, which could produce syngas with a constant H(2):CO ratio of ~2 via solar-powered CO(2) electroreduction. The generated syngas is subsequently fed into the photothermal module, which could produce high-purity CH(3)OH under 1 sun-light irradiation, with a rate of 0.238 g(CH3OH) g(cat)(-1) h(-1). This work demonstrates a feasible and sustainable route for directly converting CO(2) into high-purity CH(3)OH.