Mechanism for Generating H 2 O 2 at Water-Solid Interface by Contact-Electrification.

The recent intensification of the study of contact-electrification at water-solid interfaces and its role in physicochemical processes lead to the realization that electron transfers during water-solid contact-electrification could drive chemical reactions. This mechanism, named contact-electro-catalysis (CEC), allows chemically inert fluorinated polymers to act like single electrode electrochemical systems. This study shows hydrogen peroxide (H 2 O 2 ) is generated from air and deionized water, by ultrasound driven CEC, using fluorinated ethylene propylene (FEP) as the catalyst. For a mass ratio of catalyst to solution of 1:10000, at 20°C, the kinetic rate of H 2 O 2 evolution reaches 58.87 mmol L -1 g cat -1 h -1 . Electron paramagnetic resonance (EPR) shows electrons are emitted in the solution by the charged FEP, during ultrasonication. EPR and isotope labelling experiments show H 2 O 2 is formed from hydroxyl radicals (HO • ) or two superoxide radicals (O 2 •- ) generated by CEC. Finally, it is traditionally believed such radicals migrate in the solution by Brownian diffusion prior to reactions. However, Ab-initio molecular dynamic calculations reveals the radicals can react by exchanging protons and electrons through the hydrogen bonds network of water, i.e., owing to the Grotthuss mechanism. This mechanism could be relevant to other systems, artificial or natural, generating H 2 O 2 from air and water. This article is protected by copyright. All rights reserved.