Hydrophilic/Hydrophobic Composite Catalysts to Enhance Contact‐Electro‐Catalytic Performance of Polytetrafluoroethylene

Abstract The strong hydrophobicity of polytetrafluoroethylene (PTFE) restricts its effective interaction with aqueous media, thereby hindering its contact‐electro‐catalytic (CEC) performance. Herein, an effective strategy is proposed to enhance CEC efficiency by developing hydrophobic/hydrophilic composites. This approach not only improves hydrophilicity to facilitate solid–liquid contact‐electrification (CE) but also leverages solid–solid CE, significantly boosting the CEC activity of PTFE. Notably, the boron nitride (BN)/PTFE composite demonstrates exceptional CEC performance, achieving a hydrogen yield of 15.73 mmol g⁻¹ h⁻¹ in pure water, and a nitrogen reduction rate of 17.25 mmol g⁻¹ h⁻¹ in water/methanol system, far surpassing previously reported piezocatalysts and piezo‐photocatalysts. Experimental and theoretical results jointly reveal significant electron transfer between PTFE and water, as well as PTFE and BN. This work not only opens new avenues for developing high‐performance CEC materials but also provides a mechanistic framework for understanding interfacial charge‐transfer dynamics in CEC systems.