Janus electrocatalytic flow-through membrane enables highly selective singlet oxygen production

Abstract

AbstractThe importance of singlet oxygen (1O2) in the environmental and biomedical fields has motivated research for effective 1O2 production. Electrocatalytic processes hold great potential for highly-automated and scalable 1O2 synthesis, but they are energy- and chemical-intensive. Herein, we present a Janus electrocatalytic membrane realizing ultra-efficient 1O2 production (6.9 mmol per m3 of permeate) and very low energy consumption (13.3 Wh per m3 of permeate) via a fast, flow-through electro-filtration process without the addition of chemical precursors. We confirm that a superoxide-mediated chain reaction, initiated by electrocatalytic oxygen reduction on the cathodic membrane side and subsequently terminated by H2O2 oxidation on the anodic membrane side, is crucial for 1O2 generation. We further demonstrate that the high 1O2 production efficiency is mainly attributable to the enhanced mass and charge transfer imparted by nano- and micro-confinement effects within the porous membrane structure. Our findings highlight a new electro-filtration strategy and an innovative reactive membrane design for synthesizing 1O2 for a broad range of potential applications including environmental remediation.