Precise Regulation of D-Band Centers Inducing to High-Efficiency Dual-Channel Piezocatalytic H₂O₂ Production

Piezocatalysis is a promising and eco-friendly technology for hydrogen peroxide (H₂O₂) synthesis; however, its efficiency is limited by the limited active sites and slow kinetics. Herein, a novel strategy is reported that achieves spatial separation of oxidation/reduction sites by precisely tuning the d-band center, enabling efficient H₂O₂ production via dual-channel path. Results illustrate that carbon shell engineering induces an upshift in the d-band center of CdS (C@CdS), which optimizes the adsorption free energy of key intermediates (*OOH) and consequently reduces the energy barrier of H₂O₂ formation by two-electron oxygen reduction reaction (2e^- ORR). Additionally, the carbon shell not only enhances piezoelectric response and strain-mediated charge separation, but also provides oxidation sites facilitating H₂O₂ generation through water oxidation reaction (WOR). The optimized catalyst (C_0.01@CdS) demonstrates outstanding performance, attaining a remarkable H₂O₂ production rate of 1481.4 µmol g^-1 h^-1 in a pure water/air system. Moreover, C_0.01@CdS demonstrates superior degradation efficiency for persistent micropollutants under stirred conditions (1000 rpm) when incorporated into the composite membrane (C_0.01@CdS/PVDF). This work pioneers a green route for efficient piezocatalytic H₂O₂ synthesis while establishing a dual-functional platform for effective pollutant remediation. © 2025 Wiley-VCH GmbH.