Electrochemical Oxidation of Organic Compounds Induced by Electro‐Generated Free Hydroxyl Radicals on BDD Electrodes

Kapałka, Agnieszka; Baltruschat, Helmut; Comninellis, Christos

doi:10.1002/9781118062364.ch10

Cited by 14 publications

(11 citation statements)

References 14 publications

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“…The CV of BDD with NaClO4 shows the expected large onset potential for O2(g) evolution of 2.4 V vs SHE. 71 With Clpresent, the current onset potential shifts down to 2.1 V vs SHE due to the lower overpotential for Cl2(g) evolution. See Table S1 for a list of relevant thermodynamic standard and formal potentials for these reactions.…”

Section: Reactive Chlorine Species Scavenged By Ureamentioning

confidence: 99%

Selective oxidation of pharmaceuticals and suppression of perchlorate formation during electrolysis of fresh human urine

et al. 2021

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Section: Reactive Chlorine Species Scavenged By Ureamentioning

confidence: 99%

Selective oxidation of pharmaceuticals and suppression of perchlorate formation during electrolysis of fresh human urine

et al. 2021

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“…Figure1a, b shows cyclic voltammograms (CV) of oxidative sweeps of these three solutions on BDD and IrO 2 . The CV of BDD with NaClO 4 shows the expected large onset potential for O 2 (g) evolution of 2.4 V vs SHE 71. With Clpresent, the current onset potential shifts down to…”

mentioning

confidence: 91%

Oxidant Scavenging Properties of Urea Enable Selective Oxidation of Pharmaceuticals and Suppression of Oxyhalide Formation during Electrolysis of Fresh Human Urine

Clark¹,

Yang²,

Nc³

et al. 2020

Preprint

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Many pharmaceutical compounds are excreted unchanged or as active metabolites that pass through conventional wastewater treatment processes, presenting a risk to aquatic ecosystems and humans. Advanced oxidation processes (AOPs) are able to degrade these compounds but often lead to the formation of oxidation byproducts (OBPs) including chlorate, perchlorate, and halogenated organics at hazardous concentrations. Point-source remediation is desirable as it provides an avenue to destroy pharmaceuticals before dilution with wastewater. However, the high concentration of urea and chloride in fresh human suggests low selectivity of pharmaceutical oxidation and high OBP formation are likely. Here, we show that the high urea content of fresh human urine suppresses the formation of oxychloride byproducts by inhibiting formation of HOCl/OCl‒ during electrolysis, while still enabling the oxidation of pharmaceuticals by •OH due to the slow rate of urea oxidation by hydroxyl radicals. This (primarily indirect) electrochemical oxidation scheme is shown to degrade cyclophosphamide and sulfamethoxazole with surface-area-to-volume-normalized pseudo-first-order observed rate constants greater than 0.08 cm/min in authentic fresh human urine matrixes. It results in two orders-of-magnitude decrease in pharmaceutical concentrations in 2 hours while generating three orders-of-magnitude lower oxychloride byproduct concentrations in synthetic fresh urine as compared to synthetic hydrolyzed aged urine matrixes. Importantly, this proof-of-principle shows that simple and safe electrochemical methods can be used for point-source-remediation of pharmaceuticals in fresh human urine (before dilution with other wastewater) without formation of significant oxychloride byproducts.

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“…Hydroxyl radicals produced on the BDD anode surface quickly recombine to form water and oxygen during their diffusion away from the BDD anode surface. The hydroxyl radical concentration decreases by 50% at 20 nm and by 85% at 200 nm from the anode surface (Figure 2) [12]. Thus, organic oxidation reactions are limited to the reaction zone, approximately 20 nm from the anode surface.…”

Section: Introduction Of Retardation Factormentioning

confidence: 97%

“…These characteristics significantly decrease oxygen formation from the recombination of radicals generated by water electrolysis, and they create a wide potential window for the oxidation reactions between radicals and organic compounds. For example, the hydroxyl concentration near the BDD surface can be maintained at 7.0 × 10 −5 mol•dm −3 at a current density of 300 A•m −2 , which is about 10 6 times higher than the hydroxyl concentrations in the hydrogen peroxide oxidation processes [4,[10][11][12]. These findings have generated ample interest in the application of BDD anode.…”

Section: Introductionmentioning

confidence: 99%

Modeling and Experimental Study of Electrochemical Oxidation of Organics on Boron-Doped Diamond Anode

Xu¹

2016

CNL Nuclear Review

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Electrochemical Oxidation of Organic Compounds Induced by Electro‐Generated Free Hydroxyl Radicals on BDD Electrodes

Cited by 14 publications

References 14 publications

Selective oxidation of pharmaceuticals and suppression of perchlorate formation during electrolysis of fresh human urine

Selective oxidation of pharmaceuticals and suppression of perchlorate formation during electrolysis of fresh human urine

Oxidant Scavenging Properties of Urea Enable Selective Oxidation of Pharmaceuticals and Suppression of Oxyhalide Formation during Electrolysis of Fresh Human Urine

Modeling and Experimental Study of Electrochemical Oxidation of Organics on Boron-Doped Diamond Anode

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