Abstract

Synergy between the intrinsic photon and thermal effects from full-spectrum sunlight for H2 production is considered to be central to further improve solar-driven H2 production. To that end, the photo-thermo-catalyst that demonstrates both photoelectronic and photothermal conversion capabilities have drawn much attention recently. Here, we propose a novel synergistic full-spectrum photo-thermo-catalysis technique for high-efficient H2 production by solar-driven methanol steam reforming (MSR), along with the Pt-CuOx photo-thermo-catalyst featuring Pt-Cu/Cu2O/CuO heterojunctions by Pt-mediated in-situ photoreduction of CuO. The results show that the H2 production performance rises superlinearly with increasing light intensity. The optimal H2 production rate of 1.6 mol g−1 h−1 with the corresponding solar-to-hydrogen conversion efficiency of 7% and the CO selectivity of 5% is achieved under 15 × sun full-spectrum irradiance (1 × sun = 1 kW m−2) at 180 °C, which is much more efficient than the previously-reported Cu-based thermo-catalysts for MSR normally operating at 250∼350 °C. These attractive performances result from the optimized reaction kinetics in terms of intensified intermediate adsorption and accelerated carrier transfer by long-wave photothermal effect, and reduced activation barrier by short-wave photoelectronic effect, due to the broadened full-spectrum absorbability of catalyst. This work has brought us into the innovative technology of full-spectrum synergistic photo-thermo-catalysis, which is envisioned to expand the application fields of high-efficient solar fuel production.

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