While morphology regulation in conventional catalysis mainly increases the specific surface area to expose more active sites, in piezocatalysis, it additionally alters the polarization properties of the materials. In this work, by leveraging the dual benefit of morphology regulation in piezocatalysis, we used cetyltrimethylammonium bromide (CTAB) to synthesize two-dimensional ultrathin Bi₂WO₆ (BWO) nanosheets, whose minimal thickness of ~2.26 nm results from the selective adsorption of CTAB inhibiting molecular layer stacking. This morphological control not only increased the specific surface area by more than doubling from 14.47 to 29.15 m²∙g⁻¹ but also enhanced the interfacial polarization by 18.34 mV. Consequently, the effective piezoelectric coefficient of CTAB-modified BWO rose from ~10.01 to ~27.53 pm∙V⁻¹. The modified catalyst, by simultaneously increasing reactive sites and boosting piezoelectric performance, achieves a maximum per-unit-power hydrogen production rate of 61.20 μmol∙g^‒1∙h^‒1∙W^‒1, which is one of the highest values ever reported. This work demonstrates a synergistic strategy of morphology engineering to enhance the surface reactivity and piezoelectric response, offering a new paradigm for high-performance piezocatalysts.

Balancing the piezoelectric coefficient and carrier concentration of materials is key in the field of piezocatalysis. In this work, Bi₂WO₆ material with both piezoelectric and semiconductor properties was chosen as a model material. A one-step ethylene glycol (EG)-assisted solvothermal method was used to synthesize Bi₂WO₆ with oxygen vacancies. By controlling the solvothermal time and temperature, the oxygen vacancy concentration (C_OV) was regulated. As C_OV increases, the piezoelectric coefficient decreases, the carrier concentration increases, and the hydrogen production rate first increases but then decreases. When C_OV reaches 1.45×10¹² spins·mg⁻¹, the corresponding piezoelectric coefficient and carrier concentration are 13.9 pm·V⁻¹ and 2.90×10²⁰ cm⁻³, respectively. The optimal hydrogen production rate per power of 2.21 μmol·g⁻¹·h⁻¹·W⁻¹ is equivalent to or even better than that of most reported piezocatalysts. The piezoelectric coefficient and carrier concentration, as two factors, jointly determine the piezocatalytic performance. The findings of this research can provide important and deep-seated insights for better piezocatalysts in the future.