Abstract
Sono-photo-catalysis (SPC) has been regarded as a promising route for hydrogen evolution from water splitting due to the sono-photo-synergism, whereas its current performance (∼μmol g-1 h-1) is yet far from expectation. Herein, we give the first demonstration that the intrinsically coupled thermal effects of light and ultrasound, which is normally underestimated or neglected, can simultaneously reshape the photo- and sono-catalytic activities for hydrogen evolution and establish a higher degree of synergy between light and ultrasound in SPC even on the traditional Pt-TiO2 catalyst. A high-efficient hydrogen evolution rate of 225.04 mmol g-1 h-1 with light-to‑hydrogen efficiency of 0.89% has been achieved in thermally-enhanced SPC, which is an order of magnitude higher than that without thermal effects. More impressively, the increase of synergy index up to 53% has been achieved. Through experiments and theoretical calculations, the thermally-enhanced sono-photo-synergism is attributed to the sono-photo-thermo-modulated structural optimization of defect-rich TiO2 support and deaggregated Pt species with functional complementary lattice facets, which optimizes not only the thermodynamic properties by enhancing light harvesting and the charge redox power, but also the kinetic properties by accelerating the net efficiency of charge separation and the whole processes of water splitting, including the dissociation of water molecules on high-index (200) Pt facets and production of H∗ intermediates on defect-rich TiO2-x support and low-index (111) Pt facets. This study exemplifies that coupling light- and ultrasonic-induced thermal effects in SPC system could enhance the synergy between light and ultrasound by modulating catalyst structure to achieve double optimization of thermodynamic and kinetic properties of SPC hydrogen evolution.