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1.
Proc Natl Acad Sci U S A ; 121(7): e2315688121, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38315857

RESUMO

Integrating reactive radicals into membranes that resemble biological membranes has always been a pursuit for simultaneous organics degradation and water filtration. In this research, we discovered that a radical polymer (RP) that can directly trigger the oxidative degradation of sulfamethozaxole (SMX). Mechanistic studies by experiment and density functional theory simulations revealed that peroxyl radicals are the reactive species, and the radicals could be regenerated in the presence of O2. Furthermore, an interpenetrating RP network membrane consisting of polyvinyl alcohol and the RP was fabricated to demonstrate the simultaneous filtration of large molecules in the model wastewater stream and the degradation of ~ 85% of SMX with a steady permeation flux. This study offers valuable insights into the mechanism of RP-triggered advanced oxidation processes and provides an energy-efficient solution for the degradation of organic compounds and water filtration in wastewater treatment.

2.
Proc Natl Acad Sci U S A ; 120(43): e2311585120, 2023 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-37844255

RESUMO

Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure-performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure-reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.

3.
Proc Natl Acad Sci U S A ; 119(30): e2202682119, 2022 07 26.
Artigo em Inglês | MEDLINE | ID: mdl-35858430

RESUMO

Heterogeneous peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have shown a great potential for pollutant degradation, but their feasibility for large-scale water treatment application has not been demonstrated. Herein, we develop a facile coprecipitation method for the scalable production (∼10 kg) of the Cu-Fe-Mn spinel oxide (CuFeMnO). Such a catalyst has rich oxygen vacancies and symmetry-breaking sites, which endorse it with a superior PMS-catalytic capacity. We find that the working reactive species and their contributions are highly dependent on the properties of target organic pollutants. For the organics with electron-donating group (e.g., -OH), high-valent metal species are mainly responsible for the pollutant degradation, whereas for the organics with electron-withdrawing group (e.g., -COOH and -NO2), hydroxyl radical (•OH) as the secondary oxidant also plays an important role. We demonstrate that the CuFeMnO-PMS system is able to achieve efficient and stable removal of the pollutants in the secondary effluent from a municipal wastewater plant at both bench and pilot scales. Moreover, we explore the application prospect of this PMS-based AOP process for large-scale wastewater treatment. This work describes an opportunity to scalably prepare robust spinel oxide catalysts for water purification and is beneficial to the practical applications of the heterogeneous PMS-AOPs.


Assuntos
Óxido de Alumínio , Óxido de Magnésio , Peróxidos , Poluentes da Água , Purificação da Água , Óxido de Alumínio/química , Catálise , Óxido de Magnésio/química , Peróxidos/química , Poluentes da Água/química , Purificação da Água/métodos
4.
Small ; : e2311691, 2024 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-38440836

RESUMO

With maximum utilization of active metal sites, more and more researchers have reported using single atom catalysts (SACs) to activate persulfate (PS) for organic pollutants removal. In SACs, single metal atoms (Fe, Co, Cu, Mn, etc.) and different substrates (porous carbon, biochar, graphene oxide, carbon nitride, MOF, MoS2 , and others) are the basic structural. Metal single atoms, substances, and connected chemical bonds all have a great influence on the electronic structures that directly affect the activation process of PS and degradation efficiency to organic pollutants. However, there are few relevant reviews about the interaction between metal single atoms and substances during PS activation process. In this review, the SACs with different metal species and substrates are summarized to investigate the metal-support interaction and evaluate their effects on PS oxidation reaction process. Furthermore, how metal atoms and substrates affect the reactive species and degradation pathways are also discussed. Finally, the challenges and prospects of SACs in PS-AOPs are proposed.

5.
Environ Sci Technol ; 58(13): 6030-6038, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38517061

RESUMO

Increasing radical yields to reduce UV fluence requirement for achieving targeted removal of micropollutants in water would make UV-based advanced oxidation processes (AOPs) less energy demanding in the context of United Nations' Sustainable Development Goals and carbon neutrality. We herein demonstrate that, by switching the UV radiation source from conventional low-pressure UV at 254 nm (UV254) to emerging Far-UVC at 222 nm (UV222), the fluence-based concentration of HO• in the UV/peroxydisulfate (UV/PDS) AOP increases by 6.40, 2.89, and 6.00 times in deionized water, tap water, and surface water, respectively, with increases in the fluence-based concentration of SO4•- also by 5.06, 5.81, and 55.47 times, respectively. The enhancement to radical generation is confirmed using a kinetic model. The pseudo-first-order degradation rate constants of 16 micropollutants by the UV222/PDS AOP in surface water are predicted to be 1.94-13.71 times higher than those by the UV254/PDS AOP. Among the tested water matrix components, chloride and nitrate decrease SO4•- but increase HO• concentration in the UV222/PDS AOP. Compared to the UV254/PDS AOP, the UV222/PDS AOP decreases the formation potentials of carbonaceous disinfection byproducts (DBPs) but increases the formation potentials of nitrogenous DBPs.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Água , Fotólise , Poluentes Químicos da Água/análise , Peróxido de Hidrogênio , Oxirredução , Raios Ultravioleta , Desinfecção
6.
Environ Sci Technol ; 2024 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-38334031

RESUMO

Recently, reactive cobalt (Co) species, including Co(IV)-oxo and Co(II)-OOSO3- complexes, were proposed to be the primary intermediates formed during the process of activating peroxymonosulfate (PMS) by Co(II), mainly based on the observation that the methyl phenyl sulfoxide (MPSO) probe was transformed to methyl phenyl sulfone (MPSO2) in this process. However, in this work, we rationalized the results of the MPSO probe assay based on the chemistry of aqueous Co(III), an alternative reactive Co species. Moreover, 18O-labeled water experiments and Raman spectroscopy analysis clearly proved the Co(III) formation in the Co(II)/PMS system. In parallel, sulfate radicals (SO4•-) and hydroxyl radicals (HO•) were also involved in this system. Further, the relative contribution of Co(III) to the abatement of carbamazepine (CBZ), a representative micropollutant, in the Co(II)/PMS system was significantly increased by increasing the Co(II) dosage but was dramatically decreased by improving the PMS dosage and increasing the pH from 3 to 7. Additionally, the degradation pathway of CBZ by Co(III) and the Co(II)/PMS system was comparatively explored, confirming that Co(III) participated in the hydroxylation, carbonylation, deacetylation, and ring reduction of CBZ by the Co(II)/PMS system. Our work addresses the controversy regarding the reactive Co species involved in the Co(II)/PMS system with evidence of Co(III) as the chief one, which highlights the significance of re-evaluating the relative contribution of Co(III) in relevant environmental decontamination processes.

7.
Environ Sci Technol ; 58(4): 2123-2132, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38237556

RESUMO

Advanced oxidation processes (AOPs) often employ strong oxidizing inorganic radicals (e.g., hydroxyl and sulfate radicals) to oxidize contaminants in water treatment. However, the water matrix could scavenge the strong oxidizing radicals, significantly deteriorating the treatment efficiency. Here, we report a periodate/catechol process in which reactive quinone species (RQS) including the o-semiquinone radical (o-SQ•-) and o-benzoquinone (o-Q) were dominant to effectively degrade anilines within 60 s. The second-order reaction rate constants of o-SQ•- and o-Q with aniline were determined to be 1.0 × 108 and 4.0 × 103 M-1 s-1, respectively, at pH 7.0, which accounted for 21% and 79% of the degradation of aniline with a periodate-to-catechol molar ratio of 1:1. The major byproducts were generated via addition or polymerization. The RQS-based process exhibited excellent anti-interference performance in the degradation of aniline-containing contaminants in real water samples in the presence of diverse inorganic ions and organics. Subsequently, we extended the RQS-based process by employing tea extract and dissolved organic matter as catechol replacements as well as metal ions [e.g., Fe(III) or Cu(II)] as periodate replacements, which also exhibited good performance in aniline degradation. This study provides a novel strategy to develop RQS-based AOPs for the highly selective degradation of aniline-containing emerging contaminants.


Assuntos
Compostos Férricos , Ácido Periódico , Poluentes Químicos da Água , Peróxido de Hidrogênio , Oxirredução , Benzoquinonas , Compostos de Anilina , Catecóis , Poluentes Químicos da Água/análise
8.
Environ Res ; 250: 118559, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38412912

RESUMO

Tequila production in Mexico generates large quantities of agave bagasse (AB), a waste that could be used more efficiently. AB has a high cellulose, hemicellulose, and lignin content, which allows its use as a precursor for synthesizing carbonaceous materials. In the present work, the synthesis of activated carbon impregnated with Fe2+ (AG-Fe-II) and Fe3+ (AG-Fe-III) was carried out and evaluated in a hybrid adsorption-AOP (advanced oxidation process) methodology for sulfamethazine removal (SMT). The materials were characterized before and after the process to determine their morphological, textural, and physicochemical properties. Subsequently, the effect of the main operational variables (pH, initial SMT concentration, mass, and activator dosage) on the hybrid adsorption-degradation process was studied. The Fenton-like reaction was selected as the AOP for the degradation step, and potassium persulfate (K2S2O8) was used as an activating agent. The main iron crystallographic phases in AG-Fe-II were FeS, with a uniform distribution of iron particles over the material's surface. The main crystallographic phase for AG-Fe-III was Fe3O4. The hybrid process achieved 61% and 78% removal efficiency using AG-Fe-II and AG-Fe-III samples, respectively. The pH and initial SMT concentration were the most critical factors for removing SMT from an aqueous phase. Finally, the material was successfully tested in repeated adsorption-degradation cycles.


Assuntos
Agave , Carvão Vegetal , Sulfametazina , Poluentes Químicos da Água , Adsorção , Sulfametazina/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Carvão Vegetal/química , Agave/química , Purificação da Água/métodos
9.
Environ Res ; 244: 117863, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38070857

RESUMO

Metal-organic framework (MOF) and MOF-derived materials have attracted extensive research interest as environmental catalysts. In this study, a composite material (ZIF-67/CCot-8) was successfully prepared using cotton fiber as a substrate and growing ZIF-67 in situ. This material exhibited excellent catalytic performance and significantly improved the efficiency of antibiotics degradation. ZIF-67/CCot-8 at a concentration of 0.05 g/L, combined with 0.2 mM peroxymonosulfate (PMS), removed approximately 97% of ciprofloxacin (CIP) and 99% of tetracycline and sulfamethoxazole within 15 min. The high catalytic efficiency of this catalyst is mainly attributed to the uniform distribution of ZIF-67-derived nanoparticles on the surface of the cotton fibers, providing abundant active sites and thereby significantly enhancing the efficiency of antibiotics degradation. Radical quenching experiments and electron paramagnetic resonance (EPR) analyses revealed that sulfate radicals (SO4•-) and singlet oxygen (1O2) were the main active species. Mass spectrometry (MS) was used to elucidate the CIP degradation pathway. The growth of the roots and stems of soybean sprouts in different water environments (tap water, treated water, and untreated water) was also observed. The results demonstrated a significant improvement in the inhibition of plant growth in the post-degradation CIP solution, indicating a substantial reduction in the toxicity of the degraded aqueous solution. To validate the practicality of the ZIF-67/CCot-8/PMS system, a continuous-flow water-treatment device was designed. This system removed 98% of the CIP solution within 180 min, demonstrating its excellent durability. This study presents a potential pathway for effective antibiotics removal using MOF-derived materials.


Assuntos
Ciprofloxacina , Peróxidos , Ciprofloxacina/química , Peróxidos/química , Água , Antibacterianos
10.
Environ Res ; 253: 119124, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38734294

RESUMO

Polyaromatic hydrocarbons (PAHs) are the most persistent compounds that get contaminated in the soil and water. Nearly 16 PAHs was considered to be a very toxic according US protection Agency. Though its concentration level is low in the environments but the effects due to it, is enormous. Advanced Oxidation Process (AOP) is an emergent methodology towards treating such pollutants with low and high molecular weight of complex substances. In this study, sulfate radical (SO4‾•) based AOP is emphasized for purging PAH from different sources. This review essentially concentrated on the mechanism of SO4‾• for the remediation of pollutants from different sources and the effects caused due to these pollutants in the environment was reduced by this mechanism is revealed in this review. It also talks about the SO4‾• precursors like Peroxymonosulfate (PMS) and Persulfate (PS) and their active participation in treating the different sources of toxic pollutants. Though PS and PMS is used for removing different contaminants, the degradation of PAH due to SO4‾• was presented particularly. The hydroxyl radical (•OH) mechanism-based methods are also emphasized in this review along with their limitations. In addition to that, different activation methods of PS and PMS were discussed which highlighted the performance of transition metals in activation. Also this review opened up about the degradation efficiency of contaminants, which was mostly higher than 90% where transition metals were used for activation. Especially, on usage of nanoparticles even 100% of degradation could be able to achieve was clearly showed in this literature study. This study mainly proposed the treatment of PAH present in the soil and water using SO4‾• with different activation methodologies. Particularly, it emphasized about the importance of treating the PAH to overcome the risk associated with the environment and humans due to its contamination.


Assuntos
Recuperação e Remediação Ambiental , Oxirredução , Hidrocarbonetos Policíclicos Aromáticos , Sulfatos , Sulfatos/química , Sulfatos/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/química , Recuperação e Remediação Ambiental/métodos , Poluentes Ambientais/química , Poluentes Ambientais/análise
11.
Environ Res ; 253: 118947, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38744372

RESUMO

In our era, water pollution not only poses a serious threat to human, animal, and biotic life but also causes serious damage to infrastructure and the ecosystem. A set of physical, chemical, and biological technologies have been exploited to decontaminate and/or disinfect water pollutants, toxins, microbes, and contaminants, but none of these could be ranked as sustainable and scalable wastewater technology. The photocatalytic process can harmonize the sunlight to degrade certain toxins, chemicals, microbes, and antibiotics, present in water. For example, transition metal oxides (ZnO, SnO2, TiO2, etc.), when integrated into an organic framework of graphene or nitrides, can bring about more than 90% removal of dyes, microbial load, pesticides, and antibiotics. Similarly, a modified network of graphitic carbon nitride can completely decontaminate petrochemicals. The present review will primarily highlight the mechanistic aspects for the removal and/or degradation of highly concerned contaminants, factors affecting photocatalysis, engineering designs of photoreactors, and pros and cons of various wastewater treatment technologies already in practice. The photocatalytic reactor can be a more viable and sustainable wastewater treatment opportunity. We hope the researcher will find a handful of information regarding the advanced oxidation process accomplished via photocatalysis and the benefits associated with the photocatalytic-type degradation of water pollutants and contaminants.


Assuntos
Eliminação de Resíduos Líquidos , Águas Residuárias , Águas Residuárias/química , Eliminação de Resíduos Líquidos/métodos , Catálise , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Fotólise , Processos Fotoquímicos
12.
Environ Res ; 259: 119574, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38986800

RESUMO

Environmental pollution is increasing worldwide due to population and industrialization. Among the various forms of pollution, water pollution poses a significant challenge in contemporary times. In this study, we synthesized CuO-decorated montmorillonite K30 (MK30) nanosheets via a simple ultrasonication technique. The structural, morphological, compositional, and optical properties of the synthesized nanocomposites were evaluated using advanced instrumentation techniques. The morphology of CuO was cubic and cubic CuO evenly designed on the MK30, which was proved by Field Emission Scanning Electron Microscopy (FESEM). The adsorption photocatalytic activity of the synthesized cubic CuO/MK30 composites was examined through the degradation of MB under visible light irradiation. The apparent reaction rate constant of 20% CuO/MK30 was 12.5 folds higher than that of CuO. These conditions included a catalyst dosage ranging from 5 to 15 mg, a pH level ranging from to 3-11, and a pollutant concentration ranging from 5 to 20 mg/L. The optimal conditions for MB dye removal were determined using response surface methodology (RSM). A scavenger study of the composite was conducted and verified that •O2- and •OH radicals play an important role in the degradation process. This investigation addressed the process of adsorption and potential removal pathways, with a particular emphasis on the role of functional groups. The environmentally friendly CuO/MK30 nanocomposites exhibited potential as photocatalysts for efficiently absorbing and degrading MB dye and TC drug pollutants. They represent promising candidates for the treatment of industrial wastewater, aiming to mitigate the environmental threats posed by organic pollutants.

13.
Environ Res ; 257: 119292, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-38824982

RESUMO

This study developed a novel process named sulfidated zero-valent iron/peroxymonosulfate/visible light irradiation (S-mZVI/PMS/vis) for enhanced organic pollutant degradation. The S-mZVI/PMS/vis process exhibited remarkable catalytic activity, achieving a 99.6% rhodamine B (RhB) removal within 10 min. The degradation rate constant of RhB by the S-mZVI/PMS/vis process was found to be 6.49 and 79.84 times higher than that by the S-mZVI/PMS and PMS/vis processes, respectively. Furthermore, the S-mZVI/PMS/vis process worked efficiently across a wide pH range (3.0-9.0), and the result of five-cycle experiments demonstrated the excellent reusability and stability of S-mZVI. Radical quenching tests and electron paramagnetic resonance analysis indicated that ·O2-, 1O2, and h+ significantly contributed to the degradation of RhB through the S-mZVI/PMS/vis process. The visible light irradiation increased the Fe2+ concentration, improved the Fe3+/Fe2+ cycle, and consequently enhanced the PMS decomposition, reactive species production, and RhB degradation. This work offers a promising strategy to highly efficiently activate PMS for organic pollutants elimination from aqueous solutions.


Assuntos
Ferro , Luz , Peróxidos , Rodaminas , Poluentes Químicos da Água , Ferro/química , Rodaminas/química , Poluentes Químicos da Água/química , Peróxidos/química
14.
Environ Res ; 257: 119296, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-38824985

RESUMO

As the rapidly growing number of waste lithium-ion batteries (LIBs), the recycling and reutilization of anode graphite is of increasing interest. Converting waste anode graphite into functional materials may be a sensible option. Herein, a series of carbonaceous catalysts (TG) were successfully prepared using spent anode graphite calcined at various temperatures and applied for activating peroxymonosulfate (PMS) to degrade atrazine (ATZ). The catalyst obtained at 800 °C (TG-800) showed the optimum performance for ATZ removal (99.2% in 6 min). Various experimental conditions were explored to achieve the optimum efficiency of the system. In the TG-800/PMS system, free radicals (e.g., SO4·-, HO·), singlet oxygen (1O2), together with a direct electron transfer pathway all participated in ATZ degradation, and the ketonic (CO) group was proved as the leading catalytic site for PMS activation. The potential degradation routes of ATZ have also been presented. According to the toxicity assessment experiments, the toxicity of the intermediate products decreased. The reusability and universal applicability of the TG-800 were also confirmed. This research not only provides an efficient PMS activator for pollutant degradation, but also offers a meaningful reference for the recovery of waste anode graphite to develop environmentally functional materials.


Assuntos
Atrazina , Eletrodos , Grafite , Peróxidos , Atrazina/química , Grafite/química , Peróxidos/química , Catálise , Poluentes Químicos da Água/química , Poluentes Químicos da Água/análise , Herbicidas/química
15.
Environ Res ; 248: 118312, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38295971

RESUMO

Overuse of chlorinated disinfectants leads to a significant accumulation of disinfection by-products. Trichloroacetic acid (TCA) is a typical carcinogenic disinfection by-product. The efficacy of the conventional degradation process is reduced by the complex nature of its structure, causing a yearly increase in its prevalence within the ecological environment and consequent infliction of significant harm. In this paper, TCA was chosen as the research subject, Fe/Ni bimetallic nanoparticles were employed as the reducing catalyst, ZIF-8@HMON as the catalytic carrier combined with Fe/Ni nanoparticles, and peroxymonosulfate (PMS) was introduced to construct the reducing-advanced oxidation synergistic system and investigated the effect of this system on the degradation performance and degradation pathway of TCA. Various characterization techniques, including TEM, SEM, XRD, FT-IR, XPS, BET, were employed to investigate the morphology, element composition and structure of composite materials analysis. Moreover, the conditions for TCA degradation can be optimized by changing the experimental environment. The results showed that 25 mg of composite catalyst (mole ratio Fe: Ni = 1:1) and 10 mg of PMS effectively degraded TCA within 20-80 mg/L range at pH = 3 and 55 °C, achieving maximum degradation within 20 min. Finally, the potential pathways of TCA degradation were analyzed using EPR and LC-MS, and the corresponding reaction mechanisms were proposed.


Assuntos
Nanopartículas , Ácido Tricloroacético , Espectroscopia de Infravermelho com Transformada de Fourier , Peróxidos/química , Nanopartículas/química
16.
Luminescence ; 39(6): e4808, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38890122

RESUMO

The efficient degradation of organic pollutants in diverse environmental matrices can be achieved through the synergistic application of piezo-catalysis and photocatalysis. The focus of this study is on understanding the fundamental principles and mechanisms that govern the collaborative action of piezoelectric and photocatalytic materials. Piezoelectric nanomaterials, under mechanical stress, generate piezo-potential, which, when coupled with photocatalysts, enhances the generation and separation of charge carriers. The resulting cascade of redox reactions promotes the degradation of a wide spectrum of organic pollutants. The comprehensive investigation involves a variety of experimental techniques, including advanced spectroscopy and microscopy, to elucidate the intricate interplay between mechanical and photoinduced processes. The influence of key parameters, such as material composition, morphology, and external stimuli on the catalytic performance, is systematically explored. This study contributes to the increasing knowledge of environmental remediation and lays the foundation for the development of advanced technologies using piezo and photocatalysis for sustainable pollutant removal.


Assuntos
Recuperação e Remediação Ambiental , Processos Fotoquímicos , Catálise , Poluentes Ambientais/química , Nanoestruturas/química
17.
J Environ Manage ; 352: 120051, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38262282

RESUMO

With the rapid growth of the metallurgical industry, there is a significant increase in the production of metallurgical slags. The waste slags pose significant challenges for their disposal because of complex compositions, low utilization rates, and environmental toxicity. One promising approach is to utilize metallurgical slags as catalysts for treatment of refractory organic pollutants in wastewater through advanced oxidation processes (AOPs), achieving the objective of "treating waste with waste". This work provides a literature review of the source, production, and chemical composition of metallurgical slags, including steel slag, copper slag, electrolytic manganese residue, and red mud. It emphasizes the modification methods of metallurgical slags as catalysts and the application in AOPs for degradation of refractory organic pollutants. The reaction conditions, catalytic performance, and degradation mechanisms of organic pollutants using metallurgical slags are summarized. Studies have proved the feasibility of using metallurgical slags as catalysts for removing various pollutants by AOPs. The catalytic performance was significantly influenced by slags-derived catalysts, catalyst modification, and process factors. Future research should focus on addressing the safety and stability of catalysts, developing green and efficient modification methods, enhancing degradation efficiency, and implementing large-scale treatment of real wastewater. This work offers insights into the resource utilization of metallurgical slags and pollutant degradation in wastewater.


Assuntos
Poluentes Ambientais , Poluentes Químicos da Água , Águas Residuárias , Cobre , Substâncias Perigosas , Metalurgia , Oxirredução , Poluentes Químicos da Água/análise
18.
J Environ Manage ; 365: 121638, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38959766

RESUMO

In the sludge dewatering process, a formidable challenge arises due to the robust interactions between extracellular polymeric substances (EPS) and bound water. This study introduces a novel, synergistic conditioning method that combines iron (Fe2+)/peroxymonosulfate (PMS) and polyacrylamide (PAM) to significantly enhance sludge dewatering efficiency. The application of the Fe2+/PMS-PAM conditioning method led to a substantial reduction in specific filtration resistance (SFR) by 82.75% and capillary suction time (CST) by 80.44%, marking a considerable improvement in dewatering performance. Comprehensive analyses revealed that pre-oxidation with Fe2+/PMS in the Fe2+/PMS-PAM process effectively degraded EPS, facilitating the release of bound water. Subsequently, PAM enhanced the flocculation of fine sludge particles resulting from the advanced oxidation processes (AOPs). Furthermore, analysis based on the Extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory demonstrated shifts in interaction energies, highlighting the breakdown of energy barriers within the sludge and a transition in surface characteristics from hydrophilic (3.79 mJ m-2) to hydrophobic (-61.86 mJ m-2). This shift promoted the spontaneous aggregation of sludge particles. The innovative use of the Flory-Huggins theory provided insights into the sludge filtration mechanism from a chemical potential perspective, linking these changes to SFR. The introduction of Fe2+/PMS-PAM conditioning disrupted the uniformity of the EPS-formed gel layer, significantly reducing the chemical potential difference between the permeate and the water in the gel layer, leading to a lower SFR and enhanced dewatering performance. This thermodynamic approach significantly enhances our understanding of sludge dewatering and conditioning. These findings represent a paradigm shift, offering innovative strategies for sludge treatment and expanding our comprehension of dewatering and conditioning techniques.


Assuntos
Resinas Acrílicas , Ferro , Esgotos , Eliminação de Resíduos Líquidos , Esgotos/química , Ferro/química , Resinas Acrílicas/química , Eliminação de Resíduos Líquidos/métodos , Floculação , Peróxidos/química , Oxirredução , Filtração
19.
J Environ Manage ; 351: 119929, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38169262

RESUMO

The textile industry is an important economic sector; however, its wastewater generates a great impact on the environment. A heterogeneous solar Fenton (HSF) process was evaluated for denim wastewater treatment. The catalyst was obtained through ultrasonic modification of recycled polyethylene terephthalate (PET) with Fe nanoparticles (PET/NPs- Fe3O4). The SFH process was optimized using surface response methodology with a face-centered central composite design considering the effects of the hydraulic retention time (10, 25, and 40 min), hydrogen peroxide dosage (500, 1000, and 1500 mg/L), and mass of the packed catalyst (4, 6 and 8 g) on the color, COD, and turbidity removal efficiencies. The operating conditions for maximum COD removal were H2O2 541.7 mg/L, HRT 33.9 min, and PET/NPs- Fe3O4 dose 7.9 g with solar radiation. The removal of 91.2% COD, 86.2% color, 90.4% turbidity, and 81.9% TOC was obtained at 14.2 kJ/L QUva. PET modification yielded 1.6 mg Fe/g PET, and the modification method does not allow Fe leaching. The effluent obtained from the SFH process complies with the maximum permissible limits in Mexican legislation in terms of COD, TOC, turbidity, and color and allows the reuse of PET.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Eliminação de Resíduos Líquidos/métodos , Polietilenotereftalatos , Ultrassom , Peróxido de Hidrogênio , Ferro , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Catálise , Oxirredução
20.
J Environ Manage ; 353: 120179, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38295641

RESUMO

Natural soil minerals often contain numerous impurities, resulting in comparatively lower catalytic activity. Tropical soils are viewed as poor from soil organic matter, cations, and anions, which are considered the main impurities in the soil that are restricted to utilizing natural minerals as a catalyst. In this regard, the dissolved iron and hematite crystals that presented naturally in tropical soil were evaluated to activate oxidants and degrade pyrene. The optimum results obtained in this study were 73 %, and the rate constant was 0.0553 h-1 under experimental conditions [pyrene] = 300 mg/50 g, pH = 7, T = 55 °C, airflow = 260 mL/min, [Persulfate (PS)] = 1.0 g/L, and humic acid (HA) ( % w/w) = 0.5 %. The soil characterization analysis after the remediation process showed an increase in moieties and cracks of the soil aggregate, and a decline in the iron and aluminium contents. The scavengers test revealed that both SO4•- and O2•- were responsible for the pyrene degradation, while HO• had a minor role in the degradation process. In addition, the monitoring of by-products, degradation pathways, and toxicity assessment were also investigated. This system is considered an efficient, green method, and could provide a step forward to develop low-cost soil remediation for full-scale implementation.


Assuntos
Ferro , Poluentes do Solo , Ferro/química , Solo/química , Poluentes do Solo/química , Minerais/química , Pirenos , Oxidantes , Oxirredução
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