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Hydrogen is a promising fossil-fuel alternative fuel owing to itsenvironmentally neutral emissions and high energy density. However, the needfor purified water and external power are critical hindrances to implementationof hydrogen production. The present work reveals the potential to overcomethese shortcomings through piezo-photocatalysis of seawater using BaTiO3-x(BTO) nanoparticles. This material was made piezoelectrically active byannealing under different atmospheres, including O2, N2, Ar, and H2, the latterof which caused Ti4+ to Ti(4-x)+ multiple reductions and structural expansionsthat stabilized piezoelectric tetragonal BTO domains. The resultant defectequilibria combine ionic and electron effects, including Ti redox reactions,charge-compensating surface oxygen vacancy formation, and color centrealterations. Further, variety of experimental techniques revealed the effectsof reduction on the energy band structure. A strong piezoelectric effect andthe presence of self-polarization were confirmed by piezoresponse forcemicroscopy, while simulation work clarified the role of vibration on bandbending deriving from the former. The performance data contrasted H2 evolutionusing deionized (DI) water, simulated seawater, and natural seawater subjectedto photocatalysis, piezocatalysis, and piezo-photocatalysis. An efficient H2evolution rate of 132.4 micromol/g/h was achieved from DI water usingpiezo-photocatalysis for 5 h. In contrast, piezocatalysis for 2 h followed bypiezo-photocatalysis for 3 h resulted in H2 evolution rates of 100.7micromol/g/h for DI water, 63.4 micromol/g/h for simulated seawater, and 48.7micromol/g/h for natural seawater. This work provides potential new strategiesfor large-scale green H2 production using abundant natural resources withconventional piezoelectric material while leveraging the effects of ionsdissolved in seawater.

Direct Hydrogen Production from Water/Seawater by Irradiation/Vibration-Activated Using Defective Ferroelectric BaTiO3-x Nanoparticles