Contact-electro-catalysis (CEC) has emerged as a promising strategy for reactive oxygen species (ROS) generation, primarily through water oxidation reactions (WOR) and oxygen reduction reactions (ORR), forming the foundation of contact-electrodynamic therapy (CEDT). However, the high energy barrier of the ORR substantially limits the overall catalytic efficiency. Herein, we propose an alternative hydrogen peroxide (H 2 O 2 ) reduction pathway to replace the ORR pathway, enabling the spontaneous generation of hydroxyl radicals (•OH) without ultrasound assistance. Perfluorocarbon (PFC) nanoemulsions were prepared to construct a PFC-water liquidliquid interface. Contact electrification at the PFC-water interface induces interfacial electron-transfer process, wherein the PFC act as mediators by capturing electrons from hydroxide ions (OH -) and subsequently transferring them to H2O2 , thereby generating •OH. Furthermore, ultrasound can enhance •OH production by increasing the frequency of liquid-liquid contact and facilitating electron release from negatively charged PFC (PFC*) to H 2 O 2 . Importantly, we demonstrate that this H 2 O 2 -based CEC pathway represents a previously unrecognized mechanism underlying CEDT. In tumor microenvironments, where H2O2 is overexpressed, this mechanism leads to enhanced ROS production and tumor cell death. This work uncovers a hidden catalytic route within the CEDT framework and provides new insights into the application of CEC for tumor therapy.

This article is Open Access

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