Sustainable and feasible reagent-free electro-Fenton via sequential dual-cathode electrocatalysis

Electro-Fenton processes aim at producing oxidizing radicals with fewer added chemicals and residues but are still unable to completely eliminate both. This study demonstrates that a reagent-free electro-Fenton process that runs solely on oxygen and electricity can be achieved by sequential dual-cathode electrocatalysis. H₂O₂ is produced on an electrodeposited PEDOT on carbon cloth (PEDOT/CC) cathode and subsequently converted to hydroxyl radicals on a stainless-steel-mesh cathode. The dual-cathode system demonstrates efficient decolorization and total organic carbon (TOC) removal toward organic dyes at optimized cathodic potentials of -0.9 V for PEDOT/CC and -0.8 V for the stainless-steel mesh. The sequential dual-cathode process also displays high reusability, no iron leaching, high removal efficiency using air instead of oxygen, and low installation and operation costs. This work demonstrates a preeminent and commercially viable example of pollution control rendered by the "catalysis instead of chemical reagent" philosophy of green chemistry.