Precise Regulation of D‐Band Centers Inducing to High‐Efficiency Dual‐Channel Piezocatalytic H ₂ O ₂ Production

Abstract Piezocatalysis is a promising and eco‐friendly technology for hydrogen peroxide (H ₂ O ₂ ) 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 H ₂ O ₂ 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 H ₂ O ₂ 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 H ₂ O ₂ generation through water oxidation reaction (WOR). The optimized catalyst (C _0.01 @CdS) demonstrates outstanding performance, attaining a remarkable H ₂ O ₂ 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 H ₂ O ₂ synthesis while establishing a dual‐functional platform for effective pollutant remediation.