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1.
Microbiol Resour Announc ; 13(7): e0039124, 2024 Jul 18.
Artículo en Inglés | MEDLINE | ID: mdl-38949307

RESUMEN

Here, we present metagenomes from two cultures derived from an anaerobic microbial consortium used for bioremediation. One culture dechlorinates chloroform to dichloromethane, which is further mineralized to CO2. A second subculture was amended with only dichloromethane. We sought draft genomes of key microorganisms to identify metabolic potential in these consortia.

2.
Sci Total Environ ; 947: 174599, 2024 Jul 08.
Artículo en Inglés | MEDLINE | ID: mdl-38986706

RESUMEN

The global production of PVC is around 3.5 million tons each year. Unfortunately, the disposal of PVC waste releases toxic substances such as hydrochloric acid, polychlorinated dioxins, and furans, which can harm the environment. Therefore, there is an urgent need for a safe and environmentally friendly thermochemical treatment method that reduces the damage caused by HCl gas produced during PVC pyrolysis and improves the quality of pyrolysis oil. Hydrothermal treatment technology is one of the potential dechlorination strategies for PVC. However, its efficiency is reduced in the supercritical region, while the additives used result in secondary pollution and increased operating costs. This study is pioneering in its approach, aiming to produce high-quality oil with reduced chlorine through low-temperature hydrothermal treatment of PVC, all without additives. The results are promising, indicating that by administering steam at 250 °C with a 2.0-3.0 g-steam/g-feed ratio, we can significantly reduce chlorine content to 0.13 % while achieving an oil yield of up to 14.9 % from PVC. The hydrothermal process can reduce CO2 emissions by 15-43 % compared to pyrolysis methods, providing a simultaneous opportunity for carbon neutrality and resource recovery.

3.
Chemosphere ; 363: 142839, 2024 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-39019181

RESUMEN

The compound 1,2-dichloroethane (1,2-DCA), a persistent and ubiquitous pollutant, is often found in groundwater and can strongly affect the ecological environment. However, the extreme bio-impedance of C-Cl bonds means that a high energy input is needed to drive biological dechlorination. Biotechnology techniques based on microbial photoelectrochemical cell (MPEC) could potentially convert solar energy into electricity and significantly reduce the external energy inputs currently needed to treat 1,2-DCA. However, low electricity-generating efficiency at the anode and sluggish bioreaction kinetics at the cathode limit the application of MPEC. In this study, a g-C3N4/Blue TiO2-NTA photoanode was fabricated and incorporated into an MPEC for 1,2-DCA removal. Optimal performance was achieved when Blue TiO2 nanotube arrays (Blue TiO2-NTA) were loaded with graphitic carbon nitride (g-C3N4) 10 times. The photocurrent density of the g-C3N4/Blue TiO2-NTA composite electrode was 2.48-fold higher than that of the pure Blue TiO2-NTA electrode under light irradiation. Furthermore, the MPEC equipped with g-C3N4/Blue TiO2-NTA improved 1,2-DCA removal efficiency by 45.21% compared to the Blue TiO2-NTA alone, which is comparable to that of a microbial electrolysis cell. In the modified MPEC, the current efficiency reached 69.07% when the light intensity was 150 mW cm-2 and the 1,2-DCA concentration was 4.4 mM. The excellent performance of the novel MPEC was attributed to the efficient direct electron transfer process and the abundant dechlorinators and electroactive bacteria. These results provide a sustainable and cost-effective strategy to improve 1,2-DCA treatment using a biocathode driven by a photoanode.

4.
Environ Sci Technol ; 58(26): 11833-11842, 2024 Jul 02.
Artículo en Inglés | MEDLINE | ID: mdl-38910294

RESUMEN

Atomic hydrogen (H*) is a powerful and versatile reductant and has tremendous potential in the degradation of oxidized pollutants (e.g., chlorinated solvents). However, its application for groundwater remediation is hindered by the scavenging side reaction of H2 evolution. Herein, we report that a composite material (Fe0@Fe-N4-C), consisting of zerovalent iron (Fe0) nanoparticles and nitrogen-coordinated single-atom Fe (Fe-N4), can effectively steer H* toward reductive dechlorination of trichloroethylene (TCE), a common groundwater contaminant and primary risk driver at many hazardous waste sites. The Fe-N4 structure strengthens the bond between surface Fe atoms and H*, inhibiting H2 evolution. Nonetheless, H* is available for dechlorination, as the adsorption of TCE weakens this bond. Interestingly, H* also enhances electron delocalization and transfer between adsorbed TCE and surface Fe atoms, increasing the reactivity of adsorbed TCE with H*. Consequently, Fe0@Fe-N4-C exhibits high electron selectivity (up to 86%) toward dechlorination, as well as a high TCE degradation kinetic constant. This material is resilient against water matrix interferences, achieving long-lasting performance for effective TCE removal. These findings shed light on the utilization of H* for the in situ remediation of groundwater contaminated with chlorinated solvents, by rational design of earth-abundant metal-based single-atom catalysts.


Asunto(s)
Agua Subterránea , Hierro , Solventes , Contaminantes Químicos del Agua , Agua Subterránea/química , Hierro/química , Solventes/química , Contaminantes Químicos del Agua/química , Hidrógeno/química , Tricloroetileno/química , Halogenación , Restauración y Remediación Ambiental/métodos , Oxidación-Reducción , Adsorción
5.
Anal Chim Acta ; 1314: 342803, 2024 Jul 25.
Artículo en Inglés | MEDLINE | ID: mdl-38876516

RESUMEN

BACKGROUND: The detection of plasticizers in the environment is important to prevent environmental risks and people's health hazards. Improving recycling efficiency of waste PVC still faced challenges. RESULTS: In this work, it was found that solid products from waste PVC/coal gangue dechlorination in subcritical water (dPVC) had strong catalysis activity for luminol-H2O2 chemiluminescence (CL) reaction. Phthalates, common plasticizers, could bond and adsorb on dPVC, which greatly inhibited the luminol-H2O2-dPVC CL reaction. Based on this, a low-cost CL analysis was constructed for the detection of phthalates combinations (PACs) and di-(2-ethylhexyl) phthalate (DEHP) in the environment. The detection limit for PACs and DEHP was 0.048 ng/L and 0.13 ng/L, respectively. Compared with HPLC standard method, the dPVC CL analysis had accuracy and reliability for the detection of phthalates in actual environmental samples. Besides, the results of life cycle assessment (LCA) revealed that dPVC for CL sensing materials had significantly small global warming potential (GWP). SIGNIFICANCE: The use of dPVC for CL sensing not only improved the recycling efficiency of PVC, but also reduced carbon emissions of obtaining CL sensing materials.

6.
J Hazard Mater ; 475: 134825, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38876014

RESUMEN

The coupling of thermal remediation with microbial reductive dechlorination (MRD) has shown promising potential for the cleanup of chlorinated solvent contaminated sites. In this study, thermal treatment and bioaugmentation were applied in series, where prior higher thermal remediation temperature led to improved TCE dechlorination performance with both better organohalide-respiring bacteria (OHRB) colonization and electron donor availability. The 60 °C was found to be a key temperature point where the promotion effect became obvious. Amplicon sequencing and co-occurrence network analysis demonstrated that temperature was a more dominating factor than bioaugmentation that impacted microbial community structure. Higher temperature of prior thermal treatment resulted in the decrease of richness, diversity of indigenous microbial communities, and simplified the network structure, which benefited the build-up of newcoming microorganisms during bioaugmentation. Thus, the abundance of Desulfitobacterium increased from 0.11 % (25 °C) to 3.10 % (90 °C). Meanwhile, released volatile fatty acids (VFAs) during thermal remediation functioned as electron donors and boosted MRD. Our results provided temperature-specific information on synergistic effect of sequential thermal remediation and bioaugmentation, which contributed to better implementation of the coupled technologies in chloroethene-impacted sites.


Asunto(s)
Biodegradación Ambiental , Halogenación , Tricloroetileno , Tricloroetileno/metabolismo , Tricloroetileno/química , Contaminantes Químicos del Agua/metabolismo , Contaminantes Químicos del Agua/química , Calor , Ácidos Grasos Volátiles/metabolismo , Oxidación-Reducción , Desulfitobacterium/metabolismo , Temperatura , Bacterias/metabolismo , Bacterias/genética , Microbiota , Restauración y Remediación Ambiental/métodos , Cloro/química , Cloro/metabolismo
7.
ChemSusChem ; : e202400517, 2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38890556

RESUMEN

Electrosynthesis of alkyl carboxylic acids upon activating stronger alkyl chlorides at low-energy cost is desired in producing carbon-rich feedstock. Carbon dioxide (CO2), a greenhouse gas, has been recognized as an ideal primary carbon source for those syntheses as such events also mitigate the atmospheric CO2 level, which is already alarming. On the other hand, the promising upcycling of polyvinyl chloride to polyacrylate is a high energy-demanding carbon-chloride (C-Cl) bond activation process. Molecular catalysts that can efficiently perform such transformation under ambient reaction conditions are rarely known. Herein, we reveal a Ni-pincer complex that catalyzes the electrochemical upgrading of polyvinyl chloride to polyacrylate in 95% yield. The activities of such a Ni electrocatalyst bearing a redox-active ligand were also tested to convert diverse examples of unactivated alkyl chlorides to their corresponding carboxylic acid derivatives. Furthermore, electronic structure calculations revealed that CO2 binding occurs in a resting state to yield an CO2 adduct and that the C-Cl bond activation step is the rate-determining transition state, which has an activation energy of 19.3 kcal/mol. A combination of electroanalytical methods, control experiments, and computational studies were also carried out to propose the mechanism of the electrochemical C-Cl activation process with the subsequent carboxylation step.

8.
Environ Sci Technol ; 58(25): 11193-11202, 2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38859757

RESUMEN

Per- and poly fluoroalkyl substances (PFASs) are often encountered with nonaqueous phase liquid (NAPL) in the groundwater at fire-fighting and military training sites. However, it is unclear how PFASs affect the dechlorination performance of sulfidized nanoscale zerovalent iron (S-nFe0), which is an emerging promising NAPL remediation agent. Here, S-nFe0 synthesized with controllable S speciation (FeS or FeS2) were characterized to assess their interactions with PFASs and their dechlorination performance for trichloroethylene NAPL (TCE-NAPL). Surface-adsorbed PFASs blocked materials' reactive sites and inhibited aqueous TCE dechlorination. In contrast, PFASs-adsorbed particles with improved hydrophobicity tended to enrich at the NAPL-water interface, and the reactive sites were re-exposed after the PFASs accumulation into the NAPL phase to accelerate dechlorination. This PFASs-induced phenomenon allowed the materials to present a higher reactivity (up to 1.8-fold) with a high electron efficiency (up to 99%) for TCE-NAPL dechlorination. Moreover, nFe0-FeS2 with a higher hydrophobicity was more readily enriched at the NAPL-water interface and more reactive and selective than nFe0-FeS, regardless of coexisting PFASs. These results unveil that a small amount of yet previously overlooked coexisting PFASs can favor selective reductions of TCE-NAPL by S-nFe0, highlighting the importance of materials hydrophobicity and transportation induced by S and PFASs for NAPL remediation.


Asunto(s)
Hierro , Hierro/química , Contaminantes Químicos del Agua/química , Halogenación , Agua Subterránea/química
9.
Chemosphere ; 361: 142413, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38795920

RESUMEN

This study explored the degradation potential of a yeast strain, Meyerozyma caribbica, alone and in combination with Bacillus velezensis and Priestia megaterium, found novel for lindane biodegradation. Isolated from hexachlorocyclohexane (HCH)-contaminated sites, M. caribbica, B. velezensis, and P. megaterium demonstrated lindane reduction efficiencies of 86.5%, 78.6%, and 77.5%, respectively, at 750 mg L⁻1 within 10-day incubation period. Kinetic analysis revealed that M. caribbica followed the first-order degradation (r2 = 0.991; T1/2 = 4.3 days). Notably, M. caribbica exhibited the highest dechlorinase activity (9.27 U mL⁻1) in the cell supernatant. Co-cultivation as the mixed culture of M. caribbica and P. megaterium achieved maximum lindane reduction (90%) and dechlorinase activity (9.93 U mL⁻1). Whereas the mixed culture of M. caribbica and B. velezensis resulted in 80.9% reduction at 500 mg L⁻1 lindane with dechlorinase activity of 6.77 U mL⁻1. Growth kinetics, modelled using the Monod equation, showed a maximum specific growth rate of 0.416 h⁻1 for the mixed culture of M. caribbica and P. megaterium at 750 mg L⁻1 lindane. GC-MS analysis confirmed the presence of intermediate metabolites, viz., γ-pentachlorocyclohexane, 1,2,4-trichlorobenzene, 1,4-dichlorobenzene and maleyl acetate, validated successive dechlorination and oxidative-reduction processes during lindane biodegradation. The findings of the study highlighted the potential of these novel microbial strains and their mixed cultures for effective bioremediation of lindane-contamination.


Asunto(s)
Biodegradación Ambiental , Hexaclorociclohexano , Hexaclorociclohexano/metabolismo , Contaminantes del Suelo/metabolismo , Microbiología del Suelo , Insecticidas/metabolismo , Cinética , Bacillus/metabolismo
10.
Angew Chem Int Ed Engl ; 63(28): e202401972, 2024 Jul 08.
Artículo en Inglés | MEDLINE | ID: mdl-38703075

RESUMEN

Suffering from the susceptibility to decomposition, the potential electrochemical application of FeOCl has greatly been hindered. The rational design of the soft-hard material interface can effectively address the challenge of stress concentration and thus decomposition that may occur in the electrodes during charging and discharging. Herein, interlayer structure manipulation of FeOCl/MXene using soft-hard interface design method were conducted for electrochemical dechlorination. FeOCl was encapsulated in Ti3C2Tx MXene nanosheets by electrostatic self-assembly layer by layer to form a soft-hard mechanical hierarchical structure, in which Ti3C2Tx was used as flexible buffer layers to relieve the huge volume change of FeOCl during Cl- intercalation/deintercalation and constructed a conductive network for fast charge transfer. The CDI dechlorination system of FeOCl/Ti3C2Tx delivered outstanding Cl- adsorption capacity (158.47 ± 6.98 mg g-1), rate (6.07 ± 0.35 mg g-1 min-1), and stability (over 94.49 % in 30 cycles), and achieved considerable energy recovery (21.14 ± 0.25 %). The superior dechlorination performance was proved to originate from the Fe2+/Fe3+ topochemical transformation and the deformation constraint effect of Ti3C2Tx on FeOCl. Our interfacial design strategy enables a hard-to-soft integration capacity, which can serve as a universal technology for solving the traditional problem of electrode volume expansion.

11.
J Hazard Mater ; 474: 134750, 2024 Aug 05.
Artículo en Inglés | MEDLINE | ID: mdl-38820752

RESUMEN

Electrocatalytic dechlorination by atomic hydrogen (H*) is efficient, but limited by the low efficiency of H* production. Herein, a phosphorus-doped cobalt nitrogen carbon catalyst (Co-NP/C) was prepared, which had high catalytic activity in a wide pH range (3-11). The turnover frequency of Co-NP/C (3.54 min-1) was 1.21-59000 times superior to that of current Pd-based and non-noble metal catalysts (0.00006-2.92 min-1). Co-NP/C significantly enhanced H* generation, which was 1.52, 2.44, and 3.77 times stronger than that of Co-N/C, NP/C, and N/C, respectively, since the introduction of phosphorus was found enhanced the electron density of cobalt and regulated the electron transfer. Co-NP/C showed outstanding catalytic performance after ten cycles and could achieve nearly complete chloramphenicol removal. This regulation method was verified to be effective for other non-noble metal (Fe, Mn, Cu, Ni) phosphorus doped catalysts, proposing a general class for efficient electrochemical dechlorination, which would be of great significance for the elimination of chlorinated organic pollutants.

12.
Chemosphere ; 360: 142398, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38789053

RESUMEN

Both thermal and environmental processes are significant factors influencing the existing characteristics, e.g., congener distributions, and existing levels, of polychlorinated naphthalenes (PCNs) in the environment. Soil plays an important role in the life cycle of PCNs, but degradation of PCNs in soils has never been reported. In this study, we collected surface soil samples from 13 cities in the Yangtze River Delta, which is one of the most crowded areas of China and analyzed the samples for 75 PCNs. The long-range transportation from polluted areas was the major source for PCNs in remote areas, but the PCN profiles in remote areas reported in our previous studies were different from those in human settlement in this study, indicating there is a transformation of PCNs after emissions from anthropogenic activities. Two experiments were then designed to reveal the degradation mechanisms, including influencing factors, products, and pathways, of PCNs in surface soils. Based on the experiments, we found that the major factor driving the losses of PCNs in surface soils was volatilization, followed by photo irradiation and microbial metabolism. Under photo-irradiation, the PCN structures would be destroyed through a process of dechlorination followed by oxidation. In addition, the dechlorination pathways of PCNs have been established and found to be significantly influenced by the structure-related parameters.


Asunto(s)
Naftalenos , Ríos , Contaminantes del Suelo , Suelo , China , Naftalenos/química , Naftalenos/análisis , Contaminantes del Suelo/análisis , Contaminantes del Suelo/química , Suelo/química , Ríos/química , Monitoreo del Ambiente , Hidrocarburos Clorados/análisis , Hidrocarburos Clorados/química , Biodegradación Ambiental
13.
J Hazard Mater ; 472: 134438, 2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38718504

RESUMEN

Construction of an efficient bio-reductive dechlorination system remains challenging due to the narrow ecological niche and low-growth rate of organohalide-respiring bacteria during field remediation. In this study, a biochar-based organohalide-respiring bacterial agent was obtained, and its performance and effects on indigenous microbial composition, diversity, and inter-relationship in soil were investigated. A well-performing material, Triton X-100 modified biochar (BC600-TX100), was found to have the superior average pore size, specific surface area and hydrophicity, compared to other materials. Interestingly, Pseudomonas aeruginosa CP-1, which is capable of 2,4,6-TCP dechlorination, showed a 348 times higher colonization cell number on BC600-TX100 than that of BC600 after 7 d. Meanwhile, the dechlorination rate in soil showed the highest (0.732 d-1) in the BC600-TX100 bacterial agent than in the other agents. The long-term performance of the BC600-TX100 OHRB agent was also verified, with a stable dechlorination activity over six cycles. Soil microbial community analysis found the addition of the BC600-TX100 OHRB agent significantly increased the relative abundance of genus Pseudomonas from 1.53 % to 11.2 %, and Pseudomonas formed a close interaction relationship with indigenous microorganisms, creating a micro-ecological environment conducive to reductive dechlorination. This study provides a feasible bacterial agent for the in-situ bioremediation of soil contaminated organohalides. ENVIRONMENTAL IMPLICATION: Halogenated organic compounds are a type of toxic, refractory, and bio-accumulative persistent compounds widely existed in environment, widely detected in the air, water, and soil. In this study, we provide a feasible bacterial agent for the in-situ bioremediation of soil contaminated halogenated organic compounds. The application of biochar provides new insights for "Turning waste into treasure", which meets with the concept of green chemistry.


Asunto(s)
Biodegradación Ambiental , Carbón Orgánico , Clorofenoles , Microbiología del Suelo , Contaminantes del Suelo , Carbón Orgánico/química , Contaminantes del Suelo/metabolismo , Contaminantes del Suelo/química , Clorofenoles/metabolismo , Clorofenoles/química , Halogenación , Pseudomonas aeruginosa/metabolismo , Bacterias/metabolismo
14.
Sci Total Environ ; 931: 172825, 2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38692311

RESUMEN

Carbonaceous materials catalyze reductive dechlorination of chlorinated ethylenes (CEs) by iron(II) materials providing a new approach for the remediation of CE polluted groundwater. While most CEs are reduced via ß-elimination, vinyl chloride (VC), the most toxic and recalcitrant CE, degrades by hydrogenolysis. The significance of carbon catalysts for reduction of VC is well documented for iron(0) systems, but hardly investigated with iron(II) materials as reductants. In this study, a layered iron(II)­iron(III) hydroxide sulfate (green rust) was used as reductant for VC, with an N-doped graphene (NG), prepared by co-pyrolysis of graphene and urea, as catalyst. VC (80 µM) was completely reduced to ethylene within 336 h in the presence of 5 g Fe/L GR and 5 g/L NG pyrolyzed at 950 °C, following pseudo-first-order kinetics with a rate constant of 0.017 h-1. Dosing experiments demonstrated that dechlorination of VC takes place on the NG phase. Monitoring of hydrogen formation, cyclic voltammetry, and quenching experiments demonstrated that atomic hydrogen contributes significantly to the dehalogenation reaction, where NG is critical for formation of atomic hydrogen. CE competition experiments demonstrated the presence of specific VC reduction sites with hydrogenolysis being unaffected by concurrent ß-elimination reactions. The system exhibited excellent performance in natural groundwaters and in comparison with iron(0) systems. This study demonstrates that GR + NG is a promising system for remediation of VC contaminated groundwater, and the mechanistic part of the study can be used as a reference for subsequent studies.

15.
Heliyon ; 10(10): e31547, 2024 May 30.
Artículo en Inglés | MEDLINE | ID: mdl-38818155

RESUMEN

This study investigates the degradation of TCB in methanol, ethanol, hexane, and benzene solutions using gamma radiolysis. Kinetic properties of TCB dechlorination and its pathway are examined, with TCB selected as a representative chlorinated organic compound. Chromatograms of irradiated samples and mass spectra of liquid-phase products are presented. The change in concentration of TCB, dichlorobenzenes (DCB), chlorobenzene (MCB), and benzene with absorbed doses are observed. The radiation-chemical yield (G values) of TCB in the solvents are calculated as 1.83, 2.56, 1.93, and 1.84 100eV-1 in methanol, ethanol, hexane, and benzene solutions, respectively. 100 % degradation of TCB by gamma irradiation is found to be efficient in polar solvents but leads to a wide variety of byproducts in low polar solvents, particularly the formation of polychlorinated biphenyls in TCB + benzene solutions, making benzene an incompatible medium. The main dechlorination pathway of TCB involves the formation of 1,4-DCB, MCB, and benzene. Environmental Implication. The gamma irradiation of chlorinated organic compounds, focusing on TCB as a model compound, was investigated due to its status as a hazardous material for the environment and living organisms. TCB is a byproduct of the dechlorination of certain chlorinated pesticides listed under the Stockholm Convention's Persistent Organic Pollutants (POPs) list, which prohibits their production and use. Gamma irradiation was found to be an effective method for the degradation of chlorinated compounds, achieving 100 % degradation during irradiation. The study underscores the potential of gamma irradiation as a viable approach for the treatment of chlorinated compounds, particularly in addressing environmental and health concerns associated with TCB and related compounds.

16.
Environ Sci Pollut Res Int ; 31(23): 34661-34674, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38713350

RESUMEN

Rapid passivation and aggregation of nanoscale zero-valent iron (nZVI) seriously limit its performance in the remediation of different contaminants from wastewater. To overcome such issues, in the present study, nano-palladium/iron (nPd/Fe) was simultaneously improved by biochar (BC) prepared from discarded peanut shells and green complexing agent sodium citrate (SC). For this purpose, a composite (SC-nPd/Fe@BC) was successfully synthesized to remove 2,4-dichlorophenol (2,4-DCP) from wastewater. In the SC-nPd/Fe@BC, BC acts as a carrier with dispersed nPd/Fe particles to effectively prevent its agglomeration, and increased the specific surface area of the composite, thereby improving the reactivity and stability of nPd/Fe. Characterization results demonstrated that the SC-nPd/Fe@BC composites were well dispersed, and the agglomeration was weakened. The formation of the passivation layer on the surface of the particles was inhibited, and the mechanism of SC and BC improving the reactivity of nPd/Fe was clarified. Different factors were found to influence the reductive dichlorination of 2,4-DCP, including Pd loading, Fe:C, SC addition, temperature, initial pH, and initial pollutant concentration. The dechlorination results revealed that the synergistic effect of the BC and SC made the removal efficiency and dechlorination rate of 2,4-DCP by SC-nPd/Fe@BC reached to 96.0 and 95.6%, respectively, which was better than that of nPd/Fe (removal: 46.2%, dechlorination: 45.3%). Kinetic studies explained that the dechlorination reaction of 2,4-DCP and the data were better represented by the pseudo-first-order kinetic model. The reaction rate constants followed the order of SC-nPd/Fe@BC (0.0264 min-1) > nPd/Fe@BC (0.0089 min-1) > SC-nPd/Fe (0.0081 min-1) > nPd/Fe (0.0043 min-1). Thus, SC-nPd/Fe@BC was capable of efficiently reducing 2,4-DCP and the dechlorination efficiency of BC and SC synergistically assisted composite on 2,4-DCP was much better than that of SC-nPd/Fe, nPd/Fe@BC and nPd/Fe. Findings suggested that SC-nPd/Fe@BC can be promising for efficient treatment of chlorinated pollutants.


Asunto(s)
Carbón Orgánico , Clorofenoles , Hierro , Paladio , Clorofenoles/química , Paladio/química , Hierro/química , Carbón Orgánico/química , Contaminantes Químicos del Agua/química , Ácido Cítrico/química , Aguas Residuales/química
17.
Environ Res ; 252(Pt 2): 118899, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38604486

RESUMEN

The integration of electrokinetic and bioremediation (EK-BIO) represents an innovative approach for addressing trichloroethylene (TCE) contamination in low-permeability soil. However, there remains a knowledge gap in the impact of the inoculation approach on TCE dechlorination and the microbial response with the presence of co-existing substances. In this study, four 1-dimensional columns were constructed with different inoculation treatments. Monitoring the operation conditions revealed that a stabilization period (∼40 days) was required to reduce voltage fluctuation. The group with inoculation into the soil middle (Group B) exhibited the highest TCE dechlorination efficiency, achieving a TCE removal rate of 84%, which was 1.1-3.2 fold higher compared to the others. Among degraded products in Group B, 39% was ethylene. The physicochemical properties of the post-soil at different regions illustrated that dechlorination coincided with the Fe(III) and SO42- reduction, meaning that the EK-BIO system promoted the formation of a reducing environment. Microbial community analysis demonstrated that Dehalococcoides was only detected in the treatment of injection at soil middle or near the cathode, with abundance enriched by 2.1%-7.2%. The principal components analysis indicated that the inoculation approach significantly affected the evolution of functional bacteria. Quantitative polymerase chain reaction (qPCR) analysis demonstrated that Group B exhibited at least 2.8 and 4.2-fold higher copies of functional genes (tceA, vcrA) than those of other groups. In conclusion, this study contributes to the development of effective strategies for enhancing TCE biodechlorination in the EK-BIO system, which is particularly beneficial for the remediation of low-permeability soils.


Asunto(s)
Biodegradación Ambiental , Microbiología del Suelo , Contaminantes del Suelo , Tricloroetileno , Tricloroetileno/metabolismo , Contaminantes del Suelo/metabolismo , Permeabilidad , Suelo/química
18.
J Environ Manage ; 358: 120831, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38603850

RESUMEN

Municipal solid waste incineration (MSWI) fly ash contains large amounts of Ca, Si, and other elements, giving it the potential to be used as a raw material for cement production. However, fly ash often contains a high content of salts, which greatly limits its blending ratio during cement production. These salts are commonly removed via water washing, but this process is affected by the nature and characteristics of fly ash. To clarify the influence of the ash characteristics on salt removal, a total of 60 fly ash samples from 13 incineration plants were collected, characterized, and washed. The ash characterization and cluster analysis showed that the incinerator type and flue gas purification technology/process significantly influenced the ash characteristics. Washing removed a high percentage of salts from fly ash, but the removal efficiencies varied significantly from each other, with the chlorine removal efficiency ranging from 73.76% to 96.48%, while the sulfate removal efficiency ranged from 6.92% to 51.47%. Significance analysis further revealed that the salt removal efficiency varied not only between the ash samples from different incinerators, but also between samples collected at different times from the same incinerator. The high variance of the 60 ash samples during salt removal was primarily ascribed to their different mineralogical and chemical characteristics. Mineralogical analysis of the raw and washed ash samples showed that the mineralogical forms and proportion of these salts in each ash sample greatly influenced their removal. The presence of less-soluble and insoluble chloride salts (e.g., CaClOH, Ca2Al(OH)6(H2O)2Cl etc.) in fly ash significantly affected the chlorine removal efficiency. This study also found that Fe, Mn, and Al in fly ash were negatively correlated with the dechlorination efficiency of fly ash. In summary, the different physical and chemical properties of fly ash caused great discrepancies in salt removal. Consequently, it is suggested to consider the potential impact of the ash source and ash generation time on salt removal to ensure a reliable treatment efficiency for engineering applications.


Asunto(s)
Ceniza del Carbón , Incineración , Residuos Sólidos , Ceniza del Carbón/química , China , Residuos Sólidos/análisis , Sales (Química)/química
19.
Chemosphere ; 357: 141928, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38615951

RESUMEN

Polychlorinated biphenyls (PCBs) are a primary contaminant of potential concern at the Newtown Creek superfund site. Measurements of PCBs in hundreds of samples of sediment (surface and cores) within Newtown Creek and at nearby reference locations were obtained from the Remedial Investigation (RI) databases. This data set was analyzed using Positive Matrix Factorization (PMF). A weight-of-evidence approach was used to attribute the PMF-generated fingerprints to sources. The PMF analysis generated eight factors (fingerprints or sources) that represent primary sources, such as Aroclors, as well as secondary sources, including the East River and Combined Sewer Outfalls (CSOs). In addition to the high-production volume Aroclors (1016/1242, 1248, 1254, and 1260), some less-widely used Aroclors (1232 and 1268) were found in Newtown Creek sediment. Aroclor 1268 is disproportionately abundant in the deepest sediments, while PCBs likely from CSOs are relatively more abundant in surface sediment.


Asunto(s)
Arocloros , Monitoreo del Ambiente , Sedimentos Geológicos , Bifenilos Policlorados , Contaminantes Químicos del Agua , Bifenilos Policlorados/análisis , Sedimentos Geológicos/química , Contaminantes Químicos del Agua/análisis , Arocloros/análisis , Ríos/química
20.
J Colloid Interface Sci ; 668: 171-180, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38677206

RESUMEN

The effectiveness of photocatalytic molecular oxygen (O2) activation in pollutant removal relies on the targeted production of reactive oxygen species (ROS). Herein, we demonstrate the dual-pathway activation of O2 on BiOCl through zirconium (Zr) loading. The incorporation of Zr onto the surface of BiOCl not only leads to an increased generation of oxygen vacancies (OV) but also fosters a coupling between the d electrons of Zr and OV, forming dual-active sites known as Zr-oxygen vacancies (Zr-OV). Generally, OV adsorbs O2 and transfers one electron directly to form superoxide radicals (•O2-). Contrary to the conventional single-electron direct activation of O2 to form •O2-, Zr-OV exhibits more flexible coordination and superior electron-donating capabilities. It facilitates O2 conversion to peroxide radicals (O22-) and enables the subsequent generation of •O2- from O22-, significantly promotes the dechlorination and mineralization efficiency of chlorophenol under visible light. This study presents a straightforward strategy to precisely regulate ROS production by expanding pathways, shedding light on the critical role of managing ROS generation for effective pollutant purification.

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