Assessing the Use of Probes and Quenchers for Understanding the Reactive Species in Advanced Oxidation Processes

Environmental Science & Technology, Год журнала: 2023, Номер 57(13), С. 5433 - 5444

Опубликована: Март 17, 2023

Advanced oxidation processes (AOPs) are increasingly applied in water and wastewater treatment. Understanding the role of reactive species using probes quenchers is one main requirements for good process design. However, much fundamental kinetic data reactions with lacking, probably leading to inappropriate probe quencher selection dosing. In this work, second-order rate constants over 150 such as •OH, SO4•-, Cl• chemical oxidants free chlorine persulfate were determined. Some previously ill-quantified (e.g., furfuryl alcohol methyl phenyl sulfoxide certain oxidants, nitrobenzene 1,4-dioxane halogen radicals) found be kinetically favorable. The specific can guided by improved database. criteria properly choosing dosages proposed along a procedure quantifying interference from addition. limitations approaches explicated, possible solutions combination other tools) proposed. Overall, database protocols provided work benefit future research understanding radical chemistry AOPs well radical-involved processes.

Язык: Английский

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Water decontamination via nonradical process by nanoconfined Fenton-like catalysts

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Май 19, 2023

Abstract There is an urgent need to develop effective and sustainable solutions reduce water pollution. Heterogeneous Fenton-like catalysts are frequently used eliminate contaminants from water. However, the applicability of these limited due low availability reactive species (RS). Herein, nanoconfinement strategy was applied encapsulate short-lived RS at nanoscale boost utilization efficiency in reactions. The nanoconfined catalyst fabricated by assembling Co 3 O 4 nanoparticles carbon nanotube nanochannels achieve exceptional reaction rate excellent selectivity. Experiments collectively suggested that degradation attributed singlet oxygen ( 1 2 ). Density functional theory calculations demonstrated space contributes quantum mutation alters transition state lower activation energy barriers. Simulation results revealed enrichment contaminant on reduced migration distance enhanced . synergy between shell layer core-shell structure further improved selectivity towards oxidation real waters. expected provide a viable for pollution control.

Язык: Английский

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Multiple Roles of Dissolved Organic Matter in Advanced Oxidation Processes

Environmental Science & Technology, Год журнала: 2022, Номер 56(16), С. 11111 - 11131

Опубликована: Июль 7, 2022

Advanced oxidation processes (AOPs) can degrade a wide range of trace organic contaminants (TrOCs) to improve the quality potable water or discharged wastewater effluents. Their effectiveness is impacted, however, by dissolved matter (DOM) that ubiquitous in all sources. During application an AOP, DOM scavenge radicals and/or block light penetration, therefore impacting their toward contaminant transformation. The multiple ways which different types sources impact oxidative purification are critically reviewed. inhibit degradation TrOCs, but it also enhance formation and reactivity useful for elimination alter transformation pathways contaminants. An in-depth analysis highlights inhibitory effect on efficiency TrOCs based DOM's structure optical properties its oxidants as well synergistic contribution from redox transient intermediates. AOPs influence types, mechanisms, extent byproducts formation. Research needs proposed advance practical understanding how be exploited purification.

Язык: Английский

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Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(13)

Опубликована: Март 23, 2023

The peroxymonosulfate (PMS)-triggered radical and nonradical active species can synergistically guarantee selectively removing micropollutants in complex wastewater; however, realizing this on heterogeneous metal-based catalysts with single sites remains challenging due to insufficient electron cycle. Herein, we design asymmetric Co-O-Bi triple-atom Co-doped Bi2O2CO3 facilitate PMS oxidation reduction simultaneously by enhancing the transfer between sites. We propose that result an density increase Bi decrease Co sites, thereby undergoes a reaction generate SO4•- •OH at site 1O2 site. suggest synergistic effect of SO4•-, •OH, enables efficient removal mineralization without interference from organic inorganic compounds under environmental background. As result, achieves almost 99.3% sulfamethoxazole degradation 3 min k-value as high 82.95 min-1 M-1, which is superior existing reported so far. This work provides structural regulation approach control catalytic function, will guide rational Fenton-like catalysts.

Язык: Английский

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Rational Regulation of Co–N–C Coordination for High-Efficiency Generation of ¹O₂ toward Nearly 100% Selective Degradation of Organic Pollutants

Environmental Science & Technology, Год журнала: 2022, Номер 56(12), С. 8833 - 8843

Опубликована: Май 26, 2022

Single oxygen-based advanced oxidation processes (1O2-AOPs) exhibit great prospects in selective degradation of organic pollutants. However, efficient production 1O2 via tailored design catalysts to achieve contaminants remains challenging. Herein, we develop a simple strategy regulate the components and coordination Co–N–C at atomic level by adjusting Zn/Co ratio bimetallic zeolitic imidazolate frameworks (ZnxCo1-ZIFs). Zn4Co1–C demonstrates 98% removal phenol mixed phenol/benzoic acid (phenol/BA) solutions. Density functional theory calculations experiments reveal that more active CoN4 sites are generated Zn4Co1–C, which beneficial peroxymonosulfate activation generate 1O2. Furthermore, correlation between origin selectivity well-defined is systematically investigated electron paramagnetic resonance test quenching experiments. This work may provide novel insights into target pollutants complicated water matrix.

Язык: Английский

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A systematic review of industrial wastewater management: Evaluating challenges and enablers

Journal of Environmental Management, Год журнала: 2023, Номер 348, С. 119230 - 119230

Опубликована: Окт. 11, 2023

The study provides a systematic literature review (SLR) encompassing industrial wastewater management research from the past decade, examining enablers, challenges, and prevailing practices. Originating manufacturing, energy production, diverse processes, wastewater's handling is critical due to its potential impact environment public health. aims comprehend current state of management, pinpoint gaps, outline future prospects. SLR methodology involves scouring Scopus database, yielding an initial pool 253 articles. Refinement via search code leaves 101 articles, followed by abstract screening that reduces articles 79, finally 66 well-focused left for thorough full-text examination. Results underscore significance regulatory frameworks, technological innovation, sustainability considerations as cornerstones effective management. However, substantial impediments like; inadequate infrastructure, resource constraints necessity stakeholder collaboration still exist. highlights emerging domains, exemplified advanced technologies like nanotechnology bioremediation, alongside pivotal role circular economy principles in offers exhaustive view contemporary accentuating imperative all-encompassing approach integrates regulatory, technological, facets. Notably, identifies gaps opportunities forthcoming exploration, advocating interdisciplinary intensified collaboration. study's insights cater policymakers, practitioners, researchers, equipping them address challenges capitalize on prospects effectively.

Язык: Английский

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Review of characteristics, generation pathways and detection methods of singlet oxygen generated in advanced oxidation processes (AOPs)

Chemical Engineering Journal, Год журнала: 2023, Номер 468, С. 143778 - 143778

Опубликована: Май 29, 2023

Язык: Английский

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Origin of the Excellent Activity and Selectivity of a Single-Atom Copper Catalyst with Unsaturated Cu-N₂ Sites via Peroxydisulfate Activation: Cu(III) as a Dominant Oxidizing Species

Environmental Science & Technology, Год журнала: 2022, Номер 56(12), С. 8765 - 8775

Опубликована: Май 12, 2022

As an efficient active oxidant for the selective degradation of pollutants in wastewater, high-valent copper species Cu(III) with persulfate activation has attracted substantial attention some Cu-based catalysts. However, systematic study a catalyst structure and mechanism about peroxydisulfate (PDS) is challenging owing to coexistence multiple Cu structural symmetry PDS. Herein, we anchored atom two pyridinic N atoms synthesize single-atom (CuSA-NC). Experimental characterizations theoretical calculations complemented each other well because uniform atomic sites. The was identified as site, unsaturated Cu-N2 configuration more conductive PDS than saturated Cu-N4 configuration. Benefiting from generation Cu(III), CuSA-NC exhibited obvious anti-interference performance pollutant complex matrix. superior catalytic activity compared that reported catalysts good durability continuous-flow experiment further revealed potential practical applications. This work strongly deepens understanding sites under develops approach actual water purification.

Язык: Английский

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Single-Atom Fe-N₄ Sites for Catalytic Ozonation to Selectively Induce a Nonradical Pathway toward Wastewater Purification

Environmental Science & Technology, Год журнала: 2023, Номер 57(9), С. 3623 - 3633

Опубликована: Фев. 15, 2023

Nonradical oxidation has been determined to be a promising pathway for the degradation of organic pollutants in heterogeneous catalytic ozonation (HCO). However, bottlenecks are rational design catalysts selectively induce nonradicals and interpretation detailed nonradical generation mechanisms. Herein, we propose new HCO process based on single-atom iron catalysts, which Fe-N4 sites anchored carbon skeleton exhibited outstanding activity stability oxalic acid (OA) p-hydroxybenzoic (pHBA) as well advanced treatment landfill leachate secondary effluent. Unlike traditional radical oxidation, pathways surface-adsorbed atomic oxygen (*Oad) singlet (1O2) were identified. A substrate-dependent behavior was also observed. OA adsorbed catalyst surface mainly degraded by *Oad, while pHBA mostly removed O3 1O2 bulk solution. Density functional theory calculations molecular dynamics simulations revealed that one terminal atom ozone preferred bonding with central Fe-N4, subsequently inducing cleavage O-O bond near produce *Oad 1O2. These findings highlight structural an atomic-level understanding process.

Язык: Английский

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Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Environmental Science & Technology, Год журнала: 2022, Номер 56(16), С. 11707 - 11717

Опубликована: Авг. 5, 2022

Peracetic acid (PAA) serves as a potent and low-toxic oxidant for contaminant removal. Radical-mediated catalytic PAA oxidation processes are typically non-selective, rendering weakened efficacy under complex water matrices. Herein, we explored the usage of reduced graphene oxide (rGO) activation via non-radical pathway. Outperforming most systems, rGO–PAA system exhibits near-complete removal typical micropollutants (MPs) within short time (<2 min). Non-radical direct electron transfer (DET) from MPs to plays decisive role in MP degradation, where accelerated DET is achieved by higher potential reactive surface complexes. Benefitting DET, shows robust multiple matrices with low toxicity. Notably, regime, electrostatic attraction rGO both target critical prerequisite achieving efficient oxidation, depending on conditions solution pH pKa. A heatmap model building such an interaction further established guidance regulating performance DET-mediated systems. Overall, our work unveils imperative rGO-activated expanding knowledge PAA-based treatment strategies.

Язык: Английский

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