Abstract
The 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.
Highlights
The importance of singlet oxygen (1O2) in the environmental and biomedical fields has motivated research for effective 1O2 production
Fabrication and properties of Pd–Pt–ceramic membrane (CM). Due to their intrinsic electrical insulating properties and large thickness[35,36,37], CM can serve as ideal substrates for incorporating both cathodic and anodic electrodes on separate sides of CM
We investigated the contribution of direct electro-redox reactions on either side of the Pd–Pt–CM toward SMX removal via cyclic voltammetry (CV) measurements
Summary
The importance of singlet oxygen (1O2) in the environmental and biomedical fields has motivated research for effective 1O2 production. Current approaches for 1O2 production mainly include (i) photosensitization using elaborately designed photosensitizers (e.g., molecular dyes[13] or quantum nanodots14) for visible or UVA light adsorption[8,15] and (ii) enzymatic reactions (e.g., peroxidases[16] and oxygenases[17] catalysis) in biological systems, relying on rigorous pH and temperature conditions of the intracellular environment[7,18] While both approaches face challenges for industrial scale-up, electrocatalysis (EC), a highly automated and facile technology, could offer more approachable 1O2 production pathways[19,20,21]. It is critical to improving EC efficacy by eliminating the use of chemicals, significantly shortening residence time, and enhancing the Faradaic efficiency of the process
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