Boosting Photocatalytic H ₂ and H ₂ O ₂ Evolution Enabled by Surface Non‐Uniform Pyroelectric Field Derived Dielectrophoresis Effect

Abstract Photocatalytic water splitting into H 2 and H 2 O 2 presents a promising approach for converting solar energy into chemical energy. However, sluggish charge migration and unsatisfactory mass transfer restrict its activity. Herein, a photocatalytic system composed of a ZnO/Mo 2 C/polyacrylic acid hydrogel and carbonized wood, featuring surface non‐uniform pyroelectric field‐derived dielectrophoresis effect to offer a driving force for both charge and mass transfer is demonstrated. The chaotic motion of water vapor generated by the carbonized wood and the photothermal effect of Mo 2 C induce surface temperature oscillations and alter the polarization state of ZnO, resulting in a maximum 0.52 V surface non‐uniform pyroelectric field and stimulating a 108‐fold increase in dielectrophoresis force. This photocatalytic system demonstrates a 41% reduction in carrier migration barriers induced by non‐uniform pyroelectric field, alongside a local enrichment of intermediates and optimized H 2 diffusion via dielectrophoresis force, thus resulting in a record photocatalytic activity with H 2 and H 2 O 2 evolution rates of 755.5 and 626.3 µmol h −1 , respectively. A large‐area system (900 cm 2 ) is fabricated, yielding 2.5 L of H 2 and 103.05 mmol of H 2 O 2 per day under natural sunlight. This study presents promising design criteria for creating an efficient photocatalytic system focusing on energy harvesting and the production of high‐value‐added products.