Deciphering CaO-induced peroxydisulfate activation for destruction of halogenated organic pollutants in a low energy vibrational mill

Lou, Zimo; Song, Ludi; Liu, Weiqi; Wu, Shaohua; He, Feng; Yu, Jiaguo

doi:10.1016/j.cej.2021.134090

Cited by 8 publications

(4 citation statements)

References 80 publications

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“…For instance, sulfite delivers rapid dechlorination kinetics for highly chlorinated contaminants (e.g., HCB and PeCPyr) but poor reactivity for less chlorinated targets (e.g., TCB and TeCB). In fact, our previous work confirmed the high reactivity of the oxidative co-milling agent for less chlorinated aromatics . The findings in this study can help elucidate and predict the degradation reactivity of polychlorinated aromatics with various structures during MC treatment.…”

Section: Resultssupporting

confidence: 80%

“…In fact, our previous work confirmed the high reactivity of the oxidative co-milling agent for less chlorinated aromatics. 72 The findings in this study can help elucidate and predict the degradation reactivity of polychlorinated aromatics with various structures during MC treatment. Further study is needed to couple reduction with oxidation and develop compound-specific strategies.…”

Section: Structural Effects On Degradation Of Polychlorinated Aromaticsmentioning

confidence: 84%

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Sulfite as a Green Co-milling Agent for Mechanochemical Destruction of Polychlorinated Aromatics: Working Mechanism and Structural Dependence

et al. 2023

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Mechanochemical destruction of obsolete halogenated persistent organic chemicals (especially polychlorinated aromatics) has been documented as a safe non-combustion technology, but the smooth implementation of such a system still calls for an appropriate and sustainable co-milling agent. As an example, we show that Na 2 SO 3 as a co-milling agent not only achieves faster degradation rate for hexachlorobenzene (HCB) than calcium oxide (1.4-fold) and reduced iron powders (2.9-fold) with equal mass but also enables high dechlorination ratio (97.4%) after 4 h of milling in a planetary mill. With the input of mechanical energy, the mechanistic study suggests that sulfite salts suffer partial melt to generate SO 3 2− species on fresh surfaces, which attack HCB molecules via the one-electron-transfer mechanism. Detection on intermediates and characterization on milled samples demonstrate that HCB undergoes dechlorination, polymerization, and hydrogenation and finally converts to amorphous and graphitic carbons. Correlation analysis indicates that the degradation reactivity of a specific polychlorinated aromatic compound in such a system is strongly dependent on its molecular structure (e.g., substituent groups and degree of chlorination). This work provides a new insight for utilizing sulfite for green disposal of halogenated wastes.

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Section: Resultssupporting

confidence: 80%

Section: Structural Effects On Degradation Of Polychlorinated Aromaticsmentioning

confidence: 84%

Sulfite as a Green Co-milling Agent for Mechanochemical Destruction of Polychlorinated Aromatics: Working Mechanism and Structural Dependence

et al. 2023

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“…Notably, when O 2 gas was bubbled into the cathode chamber (DO = 4.8 mg L –1 ), 2,4-DCP removal efficiency for Pd/CFF cathode chamber (47.7%) was increased by 1.8 folds (Figure S11b) compared with that for deoxygenated atmosphere, which was also approximately twice of that for CFF cathode (23.8%). In addition to monochlorophenol and phenol, we also identified products of chlorinated dihydroxybenzenes ( m / z = 142.9393) generated from electrophilic hydroxylation substitution of 2,4-DCP at ortho- and para-positions, and benzoquinones ( m / z = 106.9294) (Figure S12b), whose formation was in accordance to the mechanisms for • OH-mediated oxidation . This preliminarily indicated • OH formation via MOA on Pd/CFF.…”

Section: Resultssupporting

confidence: 56%

“…In addition to monochlorophenol and phenol, we also identified products of chlorinated dihydroxybenzenes (m/z = 142.9393) generated from electrophilic hydroxylation substitution of 2,4-DCP at ortho-and para- positions, and benzoquinones (m/z = 106.9294) (Figure S12b), whose formation was in accordance to the mechanisms for • OH-mediated oxidation. 46 This preliminarily indicated OH formed by H*-mediated MOA. 47,48 Water Flow-Driven Coupling of OER and MOA.…”

Section: ■ Introductionmentioning

confidence: 89%

Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts

Wei,

Pei,

et al. 2023

Environ. Sci. Technol.

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Electrochemical advanced oxidation process (EAOP) is a promising technology for decentralized water decontamination but is subject to parasitic anodic oxygen evolution and formation of toxic chlorinated byproducts in the presence of Cl − . To address this issue, we developed a novel electrolytic process by water flow-driven coupling of anodic oxygen evolution reaction (OER) and cathodic molecular oxygen activation (MOA). When water flows from anode to cathode, O 2 produced from OER is carried by water through convection, followed by being activated by atomic hydrogen (H*) on Pd cathode to produce • OH. The water flow-driven OER/MOA process enables the anode to be polarized at low potential (1.7 V vs SHE) that is lower than that of conventional EAOP whose • OH is produced from direct water oxidation (>2.3 V vs SHE). At a flow rate of 30 mL min −1 , the process could achieve 94.8% removal of 2,4-dichlorophenol (2,4-DCP) and 71.5% removal of chemical oxygen demand (COD) within 45 min at an anode potential of 1.7 V vs SHE and cathode potential of −0.5 V vs SHE. To achieve the comparable 2,4-DCP removal performance, 4.3-fold higher energy consumption was needed for the conventional EAOP with titanium suboxide anode (anode potential of 2.9 V vs SHE), but current efficiency declined by 3.5 folds. Unlike conventional EAOP, chlorate and perchlorate were not detected in the OER/MOA process, because low anode potential <2.0 V vs SHE was thermodynamically unfavorable for the formation of chlorinated byproducts by anodic oxidation, indicated by theoretical calculations and experimental data. This study provides a proof-in-concept demonstration of water flow-driven OER/MOA process, representing a paradigm shift of electrochemical technology for water decontamination and prevention of chlorinated byproducts, making electrochemical water decontamination more efficient, more economic, and more sustainable.

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Novel calcium oxide activated peroxymonosulfate system for methylene blue removal: Identification of key influencing factors, transformation pathway and toxicity assessment

Luo,

Liu,

Huang

et al. 2024

Chemosphere

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Deciphering CaO-induced peroxydisulfate activation for destruction of halogenated organic pollutants in a low energy vibrational mill

Cited by 8 publications

References 80 publications

Sulfite as a Green Co-milling Agent for Mechanochemical Destruction of Polychlorinated Aromatics: Working Mechanism and Structural Dependence

Sulfite as a Green Co-milling Agent for Mechanochemical Destruction of Polychlorinated Aromatics: Working Mechanism and Structural Dependence

Water Flow-Driven Coupling Process of Anodic Oxygen Evolution and Cathodic Oxygen Activation for Water Decontamination and Prevention of Chlorinated Byproducts

Novel calcium oxide activated peroxymonosulfate system for methylene blue removal: Identification of key influencing factors, transformation pathway and toxicity assessment

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