Oxidative polymerization versus degradation of organic pollutants in heterogeneous catalytic persulfate chemistry

Water Research, Год журнала: 2024, Номер 255, С. 121485 - 121485

Опубликована: Март 18, 2024

Catalytic polymerization pathways in advanced oxidation processes (AOPs) have recently drawn much attention for organic pollutant elimination owing to the rapid removal kinetics, high selectivity, and recovery of carbon from wastewater. This work presents a review on regimes AOPs their applications wastewater decontamination. The mainly highlights three critical issues reactions induced by persulfate activation (Poly-PS-AOPs), including heterogeneous catalysts, pathways, properties substrates. dominant influencing factors selection reactive oxygen species, substrates are discussed detail. Moreover, we systematically demonstrate merits challenges Poly-PS-AOPs upon degradation polymer synthesis. We particularly highlight that technology could be promising treatment industrial containing heterocyclic organics synthesis polymers polymer-functionalized materials environmental energy applications.

Язык: Английский

---

High-entropy alloys catalyzing polymeric transformation of water pollutants with remarkably improved electron utilization efficiency

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 2, 2025

Abstract High-entropy alloy nanoparticles (HEA-NPs) exhibit favorable properties in catalytic processes, as their multi-metallic sites ensure both high intrinsic activity and atomic efficiency. However, controlled synthesis of uniform ensembles at the level remains challenging. This study successfully loads HEA-NPs onto a nitrogen-doped carbon carrier (HEAs) pioneers application peroxymonosulfate (PMS) activation to drive Fenton-like oxidation. The HEAs-PMS system achieves ultrafast pollutant removal across wide pH range with strong resistance real-world water interferences. Furthermore, nonradical selectively transforms phenolics into high-molecular-weight products via polymerization pathway. unique non-mineralization regime remarkably reduces PMS consumption electron utilization efficiency up 213.4%. Further DFT calculations experimental analysis reveal that Fe Co act primary complex for activation, while Ni, Cu, Pd serve charge mediators facilitate transfer. resulting PMS* complexes on HEAs possess redox potential, which drives spatially separated phenol oxidation graphene support form phenoxyl radicals, subsequently triggering formation high-molecule polymeric reactions. offers engineered catalysts treatment low oxidant emissions.

Язык: Английский

---

Oxidative Polymerization in Water Treatment: Chemical Fundamentals and Future Perspectives

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Янв. 6, 2025

For several decades, the methodology of complete destruction organic pollutants via oxidation, i.e., mineralization, has been rooted in real water treatment applications. Nevertheless, this industrially accepted protocol is far from sustainable because excessive input chemicals and/or energy as well unregulated carbon emission. Recently, there have emerging studies on removal a completely different pathway, polymerization, meaning that target undergo oxidative polymerization reactions to generate polymeric products. These collectively shown compared conventional mineralization pathway allows more efficient pollutants, largely reduced chemicals, and suppressed In review, we aim provide comprehensive examination fundamentals process, current state-of-the-art strategies for regulation both kinetic thermodynamic perspectives, resource recovery formed end, limitations process pollutant are discussed, with perspectives future studies. Hopefully, review could not only critical insight advancement polymerization-oriented technologies greener manner but also stimulate paradigm innovations low-carbon treatment.

Язык: Английский

---

Polymeric products deactivate carbon-based catalysts in catalytic oxidation reactions

Nature Water, Год журнала: 2025, Номер 3(2), С. 178 - 190

Опубликована: Янв. 17, 2025

Язык: Английский

---

High-valent metal-oxo species transformation and regulation by co-existing chloride: Reaction pathways and impacts on the generation of chlorinated by-products

Water Research, Год журнала: 2024, Номер 257, С. 121715 - 121715

Опубликована: Май 2, 2024

High-valent metal-oxo species (HMOS) have been extensively recognized in advanced oxidation processes (AOPs) owing to their high selectivity and chemical utilization efficiency. However, the interactions between HMOS halide ions sewage wastewater are complicated, leading ongoing debates on intrinsic reactive impacts remediation. Herein, we prepared three typical HMOS, including Fe(IV), Mn(V)-nitrilotriacetic acid complex (Mn(V)NTA) Co(IV) through peroxymonosulfate (PMS) activation comparatively studied with Cl

Язык: Английский

---

Direct Electron Transfer-Driven Nontoxic Oligomeric Deposition of Sulfonamide Antibiotics onto Carbon Materials for In Situ Water Remediation

Environmental Science & Technology, Год журнала: 2024, Номер 58(27), С. 12155 - 12166

Опубликована: Июнь 27, 2024

The rising in situ chemical oxidation (ISCO) technologies based on polymerization reactions have advanced the removal of emerging contaminants aquatic environment. However, despite their promise, uncertainties persist regarding effectiveness eliminating structurally complex contaminants, such as sulfonamide antibiotics (SAs). This study elucidated that oligomerization, rather than mineralization, predominantly governs SAs carbon materials/periodate system. amine groups played a crucial role forming organic radicals and subsequent coupling due to high f– index low bond orders. Moreover, highlighted robust adhesion oligomers catalyst surface, facilitated by enhanced van der Waals forces hydrophobic interactions. Importantly, plant animal toxicity assessments confirmed nontoxic nature deposited material affirming efficacy material-based ISCO treating contaminated surface water groundwater. Additionally, novel classification approach, Δlog k, was proposed differentiate kinetic control steps, providing deeper insights into quantitative structure–activity relationship (QSAR) facilitating selection optimal descriptors during oligomerization processes. Overall, these significantly enhance our understanding via demonstrate superiority C-ISCO decontamination.

Язык: Английский

---

Comprehensive Insight into the Common Organic Radicals in Advanced Oxidation Processes for Water Decontamination

Environmental Science & Technology, Год журнала: 2024, Номер 58(44), С. 19571 - 19583

Опубликована: Окт. 23, 2024

Radical-based advanced oxidation processes (AOPs) are among the most effective technologies employed to destroy organic pollutants. Compared common inorganic radicals, such as

Язык: Английский

---

Picolinic acid-mediated Mn(II) activated periodate for ultrafast and selective degradation of emerging contaminants: Key role of high-valent Mn-oxo species

Water Research, Год журнала: 2024, Номер 266, С. 122428 - 122428

Опубликована: Сен. 10, 2024

Язык: Английский

---

Pore modulation of single atomic Fe sites for ultrafast Fenton-like chemistry with amplified electron migration oxidation

Water Research, Год журнала: 2024, Номер 268, С. 122545 - 122545

Опубликована: Сен. 30, 2024

Язык: Английский

---

Photochemical Formation of Trifluoroacetic Acid: Mechanistic Insights into a Fluoxetine-Related Aryl-CF₃ Compound

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Trifluoroacetic acid (TFA) is a ubiquitous environmental contaminant; however, its sources are poorly constrained. One understudied source from the photochemical reactions of aromatic compounds containing -CF

Язык: Английский

---