“…Current approaches for 1 O 2 production mainly include (i) photosensitization using elaborately designed photosensitizers (e.g., molecular dyes 13 or quantum nanodots 14 ) 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 1 O 2 production pathways [19][20][21] . Specifically, EC enables the flexible generation of critical 1 O 2 precursors, such as hydrogen peroxide 22,23 and hypochlorite 20,24 .…”
mentioning
confidence: 99%
“…Specifically, EC enables the flexible generation of critical 1 O 2 precursors, such as hydrogen peroxide 22,23 and hypochlorite 20,24 . In addition, as an alternative to photoexcitation or chemiexcitation, EC provides efficient electro-excitation to 1 O 2 precursors, such as cathodic activation of peroxymonosulfate 21 and anodic excitation of ferrocene 25 .…”
mentioning
confidence: 99%
“…Present EC pathways rely on high dosages of precursors, which compromise the environmental sustainability of EC 26,27 . Further, for effective oxidation of target molecules by the in situ generated 1 O 2 , EC currently requires long reaction times (range of hours) and consequently consumes high electric energy 20,21 . Therefore, 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.…”
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.
“…Current approaches for 1 O 2 production mainly include (i) photosensitization using elaborately designed photosensitizers (e.g., molecular dyes 13 or quantum nanodots 14 ) 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 1 O 2 production pathways [19][20][21] . Specifically, EC enables the flexible generation of critical 1 O 2 precursors, such as hydrogen peroxide 22,23 and hypochlorite 20,24 .…”
mentioning
confidence: 99%
“…Specifically, EC enables the flexible generation of critical 1 O 2 precursors, such as hydrogen peroxide 22,23 and hypochlorite 20,24 . In addition, as an alternative to photoexcitation or chemiexcitation, EC provides efficient electro-excitation to 1 O 2 precursors, such as cathodic activation of peroxymonosulfate 21 and anodic excitation of ferrocene 25 .…”
mentioning
confidence: 99%
“…Present EC pathways rely on high dosages of precursors, which compromise the environmental sustainability of EC 26,27 . Further, for effective oxidation of target molecules by the in situ generated 1 O 2 , EC currently requires long reaction times (range of hours) and consequently consumes high electric energy 20,21 . Therefore, 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.…”
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.
“…The validated theoretical model had the potential to predict the electro-assisted adsorption performance under complex conditions. Liu, Ding, et al (2019) developed and examined an integrated wastewater treatment process (E-ACF-PMS) which combined PMS and an activated carbon fiber (ACF) electrolysis cathode to remove carbamazepine (CBZ). The E-ACF-PMS process utilized much less energy than the E-ACF-PDS process (PDS: peroxydisulfate), and ACF material maintained excellent adsorption and catalytic ability.…”
By summarizing 187 relevant research articles published in 2019, the review is focused on the research progress of physicochemical processes for wastewater treatment. This review divides into two sections, physical processes and chemical processes. The physical processes section includes three subsections , that is, adsorption, granular filtration, and dissolved air flotation, whereas the chemical processes section has five subsections , that is, coagulation/flocculation, advanced oxidation processes, electrochemical, capacitive deionization, and ion exchange.
“…But they are limited by high capital or operating cost. Over the last decade, a great deal of interest was focused on the degradation of toxic and refractory pollutants with the advanced oxidation processes (AOPs) [13][14][15]. It has been reported that zero-valent iron (Fe 0 ) as an environmental friendly, high reductive capacity and inexpensive material has been extensively applied to treatment/remediation of wastewater and could greatly enhanced the degradation efficiency of pollutants in wastewater [16][17][18].…”
Treating hydraulic fracturing flowback fluid has been receive much attention due to its high total dissolved solid and organic matter. In this study, to remove pollutants in the influent and reduce chemical oxygen demand (COD), the process of persulfate (PS) activated by Fe0 was applied in the treatment of hydraulic fracturing flowback fluid. At the optimal parameters of experimental condition (Fe0=8 g/L, PS = 12 mmol/L, pH=7.7, temperature=25°, reaction time=5 min), 93.6% COD (111.6 mg/L) was removed. Therefore, the Fe0-PS process could be proposed as a promising treatment technology for the removal of toxic and refractory hydraulic fracturing flowback fluid wastewater.
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