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1.
Artículo en Inglés | MEDLINE | ID: mdl-39340606

RESUMEN

The co-contamination of dyes and heavy metal ions often used as mordants poses potential risks to environment and public health, and is a challenging problem that needs to be solved in water treatment. Meanwhile, improving the solid-liquid separation capability of adsorbents is of great significance for the application of adsorption technology. Herein, amidation modified hollow composite microspheres were prepared using hollow glass microsphere (HGM) as matrix through hydrolysis and condensation of silane coupling agent (A-1100) and subsequent amidation reaction. The material (HGMNE) not only exhibited good adsorption performance for DB86 and Ni2+ but also had stable self-floating capability. The adsorption of DB86 by HGMNE is mainly carried out by the electrostatic interaction between positively charged quaternary amine nitrogen and negatively charged DB86, while the adsorption of Ni2+ is achieved by the carboxyl group in EDTA group through complexation interaction to adsorb Ni2+ to form Ni complex. This research not only is devoted to the utilization of HGMNE to achieve the co-removal of DB86 and Ni2+ and flexible self-floating solid-liquid separation but also verifies the feasibility and applicability of the modification method of introducing organic adsorption functional groups through amidation reaction, so as to expand the preparation path of HGM-based adsorbents.

2.
Environ Res ; 262(Pt 2): 119878, 2024 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-39222734

RESUMEN

Sodium alginate (SA) emerges as a promising adsorbent for the remediation of heavy metal-polluted wastewater. However, the systematic investigations on how and the extent to which the various compositions in real water matrices impact its performance were essential but rare when considering its use. Here, we explored the effect of common environmental factors on Cu(II) adsorption by an as-synthesized SA-based hydrogel (SAH). The result showed that high concentration of organics (above 10 mg L-1) had a negative influence on heavy metal removal (decreased by 9.45 % at least), while inorganic ion, turbidity and antibiotics at relatively low concentrations exhibited a negligible even promoting effect (increased by 9.8 % with the presence of 5 mg L-1 Nor). Based on above results and corresponding mechanism analyses, the possible applicable and unsuitable scenarios of SAH can be predicted. SAH could be a great candidate for treating heavy metal-polluted water such as river and lake water, while it is not a good option for electroplating or livestock wastewater which contains high concentration of organic matters. Besides, the operating conditions including pH (5.0 for Cu(II), 6.0 for Ni(II)), contact time (24 h), temperature (298 K) et al. were also determined. Overall, this work provides theoretical guidance and operational strategies for promoting the practical application of SA adsorbent in water treatment.

3.
Int J Biol Macromol ; 278(Pt 3): 134997, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-39181349

RESUMEN

The flocculation of dyeing wastewater generated a large amount of sludge that was often disposed as refractory hazardous waste. The resource utilization of flocculation sludge was of great significance in terms of low treatment cost of sludge, low environmental risk and high usage efficiency of reactive dyes. Herein, a flocculation sludge-derived (FSD) adsorbent was prepared via cross-linking of flocculation sludge yielding by carboxymethyl chitosan-based flocculants and dyes. FSD adsorbent had excellent selective adsorption performance for methylene blue (MB) treatment. The highest removal rate of MB and adsorption capacity of FSD adsorbent were 96.48 % and 354.7066 mg/g, attributing to its rich functional groups, negative charges and special micropore structure. FSD adsorbent owned the favorable regeneration efficiency and stability. Its removal rate of MB was still above 71.8 % after 6 regeneration-adsorption cycles. Its leaching rate of dyes was only 0.0016 mg/mg that was rather lower than common dried flocculation sludge. The adsorption processes of FSD adsorbent were complex in accordance with its characteristics, adsorption isotherms, adsorption kinetics and theoretical calculation. Multiple adsorption mechanisms were present in the treatment of dyeing wastewater by FSD adsorbent. The resource utilization of flocculation sludge, as adsorbents, was a potential candidate in field application.


Asunto(s)
Quitosano , Floculación , Azul de Metileno , Aguas del Alcantarillado , Contaminantes Químicos del Agua , Quitosano/química , Quitosano/análogos & derivados , Azul de Metileno/química , Adsorción , Aguas del Alcantarillado/química , Cinética , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/aislamiento & purificación , Purificación del Agua/métodos , Colorantes/química , Concentración de Iones de Hidrógeno , Aguas Residuales/química
4.
Environ Sci Pollut Res Int ; 31(34): 46877-46897, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38980480

RESUMEN

The research on bio-based flocculants for waste resource utilization and environmental protection has garnered significant attention. Bio-based flocculants encompass plant-based, animal-based, and microbial variants that are prepared and modified through biological, chemical, and physical methods. These flocculants possess abundant functional groups, unique structures, and distinctive characteristics. This review comprehensively discussed the removal rates of conventional pollutants and emerging pollutants by bio-based flocculants, the interaction between these flocculants and pollutants, their impact on flocculation performance in wastewater treatment, as well as their application cost. Furthermore, it described the common challenges faced by bio-based flocculants in practical applications along with various improvement strategies to address them. With their safety profile, environmental friendliness, efficiency, renewability, and wide availability from diverse sources, bio-based flocculants hold great potential for widespread use in wastewater treatment.


Asunto(s)
Floculación , Eliminación de Residuos Líquidos , Aguas Residuales , Aguas Residuales/química , Eliminación de Residuos Líquidos/métodos , Purificación del Agua/métodos
5.
Environ Res ; 258: 119416, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-38885827

RESUMEN

To address the urgent need for efficient removal of lead-containing wastewater and reduce the risk of toxicity associated with heavy-metal wastewater contamination, materials with high removal rates and easy separation must be developed. Herein, a novel organic-inorganic hybrid material based on phosphorylated magnetic chitosan (MSCP) was synthesized and applied for the selective removal of lead (II) from wastewater. From the characterization and the experimental results can be obtained that the magnetic saturation strength of MSCP reaches 14.65 emu/g, which can be separated quickly and regenerated readily, and maintains high adsorption performance even after 5 cycles, indicating that the adsorbent possesses good magnetic separation performance and durability. Also, MSCP showed high selective adsorption performance for lead in the multiple metal ions coexistence solutions at pH 6.0 and room temperature, with an adsorption coefficient SPb-MSCP of 78.85%, which was much higher than that of MSC (the SPb-MSC was 11.59%). Additionally, in the single lead system, the sorption characteristics of Pb(II) on MSCP and MCP had obvious pH-responsiveness, and their adsorption capacity increased with the increase of solution pH, reaching the maximal values of 80.19 and 72.68 mg/g, respectively. It is noteworthy that the acid resistance of MSCP with an inert layer coated on the core is significantly improved, with almost no iron leaching from MSCP over the entire acidity range, while MCP has 7.63 mg/g of iron leaching at pH 1.0. Significantly, MSCP exhibited a maximum adsorption capacity of 102.04 mg/g, which matches the Langmuir model at pH 6.0 and 298.15 K, and points to the pseudo-second-order kinetics of the chemisorption process of Pb(II) on MSCP. These findings highlight the great potential of MSCP for Pb(II) removal from aqueous solution, making it a promising solution for Pb(II) contamination in wastewater.


Asunto(s)
Quitosano , Plomo , Fosfatos , Aguas Residuales , Contaminantes Químicos del Agua , Plomo/química , Plomo/aislamiento & purificación , Quitosano/química , Aguas Residuales/química , Contaminantes Químicos del Agua/química , Adsorción , Fosfatos/química , Concentración de Iones de Hidrógeno , Eliminación de Residuos Líquidos/métodos , Purificación del Agua/métodos
6.
Environ Pollut ; 349: 123863, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38565391

RESUMEN

Microplastics (MPs) are emerging contaminants that are widely detected in drinking water and pose a potential risk to humans. Therefore, the MP removal from drinking water is a critical challenge. Recent studies have shown that MPs can be removed by coagulation. However, the coagulation removal of MPs from drinking water remains inadequately understood. Herein, the efficiency, mechanisms, and influencing factors of coagulation for removing MPs from drinking water are critically reviewed. First, the efficiency of MP removal by coagulation in drinking water treatment plants (DWTPs) and laboratories was comprehensively summarized, which indicated that coagulation plays an important role in MP removal from drinking water. The difference in removal effectiveness between the DWTPs and laboratory was mainly due to variations in treatment conditions and limitations of the detection techniques. Several dominant coagulation mechanisms for removing MPs and their research methods are thoroughly discussed. Charge neutralization is more relevant for small-sized MPs, whereas large-sized MPs are more dependent on adsorption bridging and sweeping. Furthermore, the factors influencing the efficiency of MP removal were jointly analyzed using meta-analysis and a random forest model. The meta-analysis was used to quantify the individual effects of each factor on coagulation removal efficiency by performing subgroup analysis. The random forest model quantified the relative importance of the influencing factors on removal efficiency, the results of which were ordered as follows: MPs shape > Coagulant type > Coagulant dosage > MPs concentration > MPs size > MPs type > pH. Finally, knowledge gaps and potential future directions are proposed. This review assists in the understanding of the coagulation removal of MPs, and provides novel insight into the challenges posed by MPs in drinking water.


Asunto(s)
Agua Potable , Microplásticos , Contaminantes Químicos del Agua , Purificación del Agua , Agua Potable/química , Purificación del Agua/métodos , Contaminantes Químicos del Agua/análisis , Adsorción
7.
J Hazard Mater ; 469: 133888, 2024 May 05.
Artículo en Inglés | MEDLINE | ID: mdl-38412645

RESUMEN

The sulfite (S(IV))-based advanced oxidation process (AOP) has emerged as an appealing alternative to the traditional persulfate-based AOP for the elimination of organic contaminants from diverse water matrices. In this work, a silica reinforced ZIF-67(Co) catalyst (CZS) is fabricated, characterized and tested in the activation of S(IV) for the sulfamethoxazole (SMX) degradation. The prepared CZS demonstrates superior stability and catalytic ability for the degradation of SMX compared to ZIF-67(Co) across a broad pH range. Unlike the conventional radical-dominated oxidation systems, the CZS/S(IV) system for SMX degradation operates through a non-radical mechanism, featuring high-valent Co(IV) and singlet oxygen (1O2) as the predominated reactive species. The hydroxylated Co species exposed on the CZS surface is identified as the pivotal active site, realizing the S(IV) activation through a complexation-electron transfer process, resulting in the production of various reactive intermediates. Co(II) undergoes the conversion to Co(IV) by generated HSO5-, and 1O2 predominantly originates from the intermediate SO4•-. Profiting from the highly selective oxidation capacities of Co(IV) and 1O2, the established oxidative system demonstrates a remarkable interference resistance and exhibits an exceptional decontamination performance under real-world water conditions. In short, this work provides a sustainable S(IV)-based oxidation strategy for environmental remediation via non-radical mechanism.

8.
Water Res ; 254: 121351, 2024 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-38401287

RESUMEN

The application of Fenton-like membrane reactors for water purification offers a promising solution to overcome technical challenges associated with catalyst recovery, reaction efficiency, and mass transfer typically encountered in heterogeneous batch reaction modes. This study presents a dual-modification strategy encompassing electron polarization and defect engineering to synthesize Al-doped and oxygen vacancies (OV)-enriched Co3O4 spinel catalysts (ACO-OV). This modification empowered ACO-OV with exceptional performance in activating peroxymonosulfate (PMS) for the removal of organic contaminants. Moreover, the ACO-OV@polyethersulfone (PES) membrane/PMS system achieved organic contaminant removal through filtration (with a reaction kinetic constant of 0.085 ms-1), demonstrating outstanding resistance to environmental interference and high operational stability. Mechanistic investigations revealed that the exceptional catalytic performance of this Fenton-like membrane reactor stemmed from the enrichment of reactants, exposure of reactive sites, and enhanced mass transfer within the confined space, leading to a higher availability of reactive species. Theoretical calculations were conducted to validate the beneficial intrinsic effects of electron polarization, defect engineering, and the confined space within the membrane reactor on PMS activation and organic contaminant removal. Notably, the ACO-OV@PES membrane/PMS system not only mineralized the targeted organic contaminants but also effectively mitigated their potential environmental risks. Overall, this work underscores the significant potential of the dual-modification strategy in designing spinel catalysts and Fenton-like membrane reactors for efficient organic contaminant removal.


Asunto(s)
Óxido de Aluminio , Cobalto , Electrones , Óxidos , Polímeros , Sulfonas , Óxido de Magnesio , Peróxidos
9.
J Hazard Mater ; 465: 133476, 2024 03 05.
Artículo en Inglés | MEDLINE | ID: mdl-38232546

RESUMEN

In this work, novel multifunctional cationic template copolymers with flocculation and sterilization capabilities were synthesized using a low-pressure ultraviolet (LP-UV) template polymerization method for the removal of kaolin and Escherichia coli (E. coli) from water. The influence of template agents on the structural performance of the copolymers was evaluated through characterization, which showed that template copolymer TPADM possesses a higher cationic charge density and a more complex rough surface, contributing to better flocculation performance than that of the non-template copolymer CPADM. Under optimal experimental conditions, TPADM-1 exhibited removal rates of 98.45% for kaolin and 99% for E. coli (OD600 =0.04), marginally outperforming the non-template copolymer. Simultaneously, TPADM-1 produced good adaptability to kaolin and E. coli wastewater in terms of wide pH, speculating that charge neutralization, adsorption bridging, patching, and sweeping simultaneously dominate the flocculation mechanism. Interestingly, SEM and 3D-EEM analysis confirm that the sterilization of E. coli occurs through two distinct functions: initially adsorption followed by subsequent cell membrane rupture and leakage of cellular contents, ultimately leading to cell death. This research further confirms the feasibility of the designed novel multifunctional copolymers for achieving simultaneous disinfection and turbidity removal, demonstrating practical applicability in real water treatment processes.


Asunto(s)
Compuestos de Amonio Cuaternario , Purificación del Agua , Floculación , Caolín/química , Escherichia coli , Antibacterianos , Polímeros/química , Purificación del Agua/métodos , Cationes , Desinfección
10.
Environ Res ; 232: 116271, 2023 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-37286124

RESUMEN

In this study, an advanced oxidation process with E/Ce(IV) synergistic PMS (E/Ce(IV)/PMS) was established for the efficient removal of Reactive Blue 19 (RB19). The catalytic oxidation performance of different coupling systems was examined and the synergistic effect of E/Ce(IV) with PMS in the system was substantiated. The oxidative removal of RB19 in E/Ce(IV)/PMS was excellent, achieving a removal efficiency of 94.47% and a reasonable power consumption (EE/O value was 3.27 kWh·m-3). The effect of pH, current density, Ce(IV) concentration, PMS concentration, initial RB19 concentration and water matrix on the removal efficiency of RB19 were explored. Additionally, quenching and EPR experiments showed that the solution contains different radicals such as SO4·-, HO∙ and 1O2, where 1O2 and SO4·- played key roles, but HO∙ just acted a weaker role. Ce ion trapping experiment confirmed that Ce(IV) was involved in the reaction process and played a major role (29.91%). RB19 was subject to three possible degradation pathways, and the intermediate products displayed well biochemical properties. To conclude, the degradation mechanism of RB19 was explored and discussed. In the presence of current, E/Ce(IV)/PMS performed a rapid Ce(IV)/Ce(III) cycle, continuously generating strong catalytic oxidation Ce(IV), The reactive radicals derived from the decomposition of PMS, in conjunction with Ce(IV) and direct electro-oxidation, efficiently destroyed the molecular structure of RB19 and showed an efficient removal rate.


Asunto(s)
Antraquinonas , Peróxidos , Peróxidos/química , Oxidación-Reducción , Agua
11.
J Environ Manage ; 344: 118437, 2023 Oct 15.
Artículo en Inglés | MEDLINE | ID: mdl-37343476

RESUMEN

The ecological impacts of micro(nano)plastics (MNPs) have attracted attention worldwide because of their global occurrence, persistence, and environmental risks. Increasing evidence shows that MNPs can affect soil nutrient cycling, but the latest advances on this topic have not systematically reviewed. Here, we aim to present the state of knowledge about the effects of MNPs on soil nutrient cycling, particularly of C, N, and P. Using the latest data, the present review mainly focuses on three aspects, including (1) the effects and underlying mechanisms of MNPs on soil nutrient cycling, particularly of C, N and P, (2) the factors influencing the effects of MNPs on soil nutrient cycling, and (3) the knowledge gaps and future directions. We conclude that MNPs can alter soil nutrient cycling via mediating soil nutrient availability, soil enzyme activities, functional microbial communities, and their potential ecological functions. Furthermore, the effects of MNPs vary with MNPs characteristics (i.e., polymeric type, size, dosage, and shape), chemical additives, soil physicochemical conditions, and soil biota. Considering the complexity of MNP-soil interactions, multi-scale experiments using environmental relevant MNPs are required to shed light on the effects of MNPs on soil nutrients. By learning how MNPs influence soil nutrients cycles, this review can guide policy and management decisions to safeguard soil health and ensure sustainable agriculture and land use practices.


Asunto(s)
Plásticos , Suelo , Agricultura
12.
J Hazard Mater ; 456: 131715, 2023 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-37245367

RESUMEN

Advanced oxidation processes (AOPs) using oxygen (O2) as an oxidant represent a low-cost and sustainable wastewater treatment process. Herein, a metal-free nanotubular carbon nitride photocatalyst (CN NT) was prepared to activate O2 to degrade organic contaminants. The nanotube structure allowed for sufficient O2 adsorption, while the optical and photoelectrochemical properties enabled photogenerated charge to be efficiently transferred to the adsorbed O2 to trigger the activation process. The developed CN NT/Vis-O2 system based on O2 aeration degraded various organic contaminants and mineralized 40.7% of chloroquine phosphate within 100 min. In addition, the toxicity and environmental risk of treated contaminants were reduced. Mechanistic studies suggested that the enhanced O2 adsorption capacity and fast charge transfer behavior on CN NT surface led to reactive·O2-, 1O2 and h+ generation, each of which played a distinct role in contaminants degradation. Importantly, the proposed process could overcome the interference from water matrices and outdoor sunlight, and the energy and chemical reagent savings reduced the operating cost to about 1.63 US$·m-3. Altogether, this work provides insights into the potential application of metal-free photocatalysts and green O2 activation for wastewater treatment.

13.
RSC Adv ; 13(11): 7413-7424, 2023 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-36895777

RESUMEN

As emerging contaminants, tetracyclines pose a severe threat to aquatic environments and human health. Therefore, developing efficient approaches to remove tetracyclines from water has attracted a large amount of interest. Herein, a novel core-shell structural magnetic nanoadsorbent (FSMAS) was facilely prepared by graft copolymerization of acrylamide (AM) and sodium p-styrene sulfonate (SSS) monomers on the surface of vinyl-modified Fe3O4@SiO2 (FSM). From single factor experiments, the optimal graft copolymerization conditions were concluded to be the following: initiator concentration = 1.2‰, reaction pH = 9, monomer molar ratio = 7 : 3. The surface morphology, microstructure and physicochemical properties of as-prepared FSMAS were fully evaluated by different characterization techniques, including SEM, TEM, FTIR, XPS, XRD and VSM. The adsorption performance of FSMAS towards tetracycline hydrochloride (TCH) was systematically studied by batch adsorption experiments. Results showed that the adsorption capability of the adsorbent was largely enhanced after graft copolymerization. The removal rate of TCH by FSMAS reached 95% at solution pH = 4.0, almost 10 times higher than FSM. Besides, the adsorption process of TCH by FSMAS was very efficient, 75% of pollutant could be adsorbed after only 10 minutes, attributed to the stretch of polymer chains and the strong affinity provided by abundant functional groups. Furthermore, TCH-loaded FSMAS was easily regenerated with HCl solution, the regeneration rate was higher than 80% after five adsorption-desorption cycles. Superior adsorption capability, fast solid-liquid separation speed and satisfactory reusability demonstrated the great potential of FSMAS in practical tetracycline removal.

14.
J Hazard Mater ; 447: 130760, 2023 Apr 05.
Artículo en Inglés | MEDLINE | ID: mdl-36640512

RESUMEN

Coagulation-flocculation in industrial wastewater treatment drives environmental pollution from landfilling heavy metal-laden sludge. Efficient separation of the sludge is crucial for cost-effective metal recovery. This study explored a new separation method of Cu2+, Ni2+, Zn2+ and Cr3+ via self-floating metal hydroxides assisted by hollow glass microsphere (HGM) carriers. The amount of OH- was stoichiometric to the positive charges of metal ions, mixed with 1 mg mL-1 HGM, causing metal hydroxides to attach to HGM surface via heterogeneous nucleation. The self-floating system removed 37.5% and 14.0% more metals than sedimentation at 50 and 200 mg L-1 metal concentrations. HGM additions increased the particle size of metal hydroxides by up to 12.5 times to that of HGM at 18.8 ± 1.1 µm, benefiting their solid-liquid separation. By pumping the wastewater downward in column reactor at velocities equal to or less than the self-floating sludge, 96.4% metals were removed in continuous flow. The recovery rates of HGM and metals reached 92.0 ± 2.2% and 92.7 ± 3.2%, and the concentration of the recovered metal reached 19,339 ± 394 mg L-1 for potential reutilization in industrial electroplating. This research investigated a new separation strategy based on solid self-flotation for sustainable treatment of metal-laden wastewater.

15.
Environ Res ; 216(Pt 2): 114590, 2023 01 01.
Artículo en Inglés | MEDLINE | ID: mdl-36252834

RESUMEN

Reactive red 2 (RR2) azo dye wastewater poses a serious hazard to the water environment health, so using a novel and efficient Electro- Ce(III) (E- Ce(III)) process takes on a critical significance in treating RR2 dye wastewater. In this study, the effects of a variety of single-factor conditions on RR2 removal efficiency were evaluated in depth. The results indicated that the optimal experimental conditions are as reaction temperature of 25 °C, Na2SO4 concentration of 25 mM, Ce(III) concentration of 0.3 mM, pH of 4.0, and current density of 40.0 mA/cm2. When the RR2 dye wastewater was treated for 40 min under the optimal experimental conditions, a high removal rate of 99.8% for RR2 was obtained. It is suggested that the background ion PO43- in the dye wastewater inhibits the E-Ce (III) process, whereas Cl- facilitates this process. Moreover, the yield of Ce(IV) increases with the increase of the current density. At the current density of 40.0 mA/cm2, a reasonable energy consumption of 3.85 kW h/gTOC for the process was obtained after the 3-h treatment. The effects of different degradation processes (including Direct Electrooxidation (DEO), single Ce(III), and E-Ce (III)) on RR2 removal efficiency and TOC change were compared. The types of oxidizing substances in the E-Ce (III) process were detected, and the mechanism of RR2 oxidative degradation in the E-Ce (III) process was summarized. The result suggests that the E-Ce (III) process has low power consumption. Meanwhile, in the E-Ce (III) process, free reactive Ce(IV) with strong oxidation is continuously generated, RR2 can be efficiently degraded. And the continuous cycle transformation between Ce(III) and Ce(IV) maintains the strong oxidation of the process. The contribution of free reactive Ce(IV) and DEO to RR2 degradation was obtained as 58.8% and 39.8%, respectively. The combined effect of Ce(IV) and DEO played a major role in the E-Ce (III) process, while ·OH exhibited a relatively weak effect (nearly 1.4%). RR2 was comprised of 13 major intermediates, and the biodegradability of wastewater was improved significantly after treatment, thus facilitating the further mineralization and biodegradation of the products. The E- Ce(III) process is novel, efficient, and environment-friendly, and has a large market application space, suggesting that it can be applied as an efficient, economic, and sustainable water treatment process.


Asunto(s)
Aguas Residuales , Contaminantes Químicos del Agua , Aguas Residuales/química , Colorantes/química , Naftalenosulfonatos , Compuestos Azo/química , Oxidación-Reducción , Contaminantes Químicos del Agua/análisis
16.
Environ Res ; 214(Pt 1): 113778, 2022 11.
Artículo en Inglés | MEDLINE | ID: mdl-35798271

RESUMEN

Among homogeneous catalysts, cobalt ions exhibit ultra-high persulfate activation performance. In this work, an electrically supported medium Co(II) activated peroxydisulfate synergistic process was established to eliminate organic contaminants in water. The synergistic catalytic effect was verified by comparing the oxidative degradation performance and reaction rate constant of different coupling systems. The decolorization ability of E-Co(II)-PDS on reactive black 5 (RB5) was explored, and the results showed that the removal rate of RB5 can reach 93.21% under the optimized conditions of current density of 5.71 mA/cm2, initial pH of 4, Co(II) concentration of 0.2 mM and PDS concentration of 5 mM. The effect of water matrix on the removal of RB5 was studied, and it was found that HCO3- and humic acid significantly inhibited the degradation of RB5, while Cl- and H2PO4- could effectively promote it at a certain concentration. Notably, the degradation of RB5 in E-Co(II)-PDS system achieved lower energy consumption, with an energy consumption per unit volume (EE/O) value of 0.4304 kWh·m-3. EPR test, quenching experiments and contribution rate analysis showed that the oxidation active species in E-Co(II)-PDS process were Co(III), sulfate radicals and hydroxyl radicals, and their oxidation contribution rates were 15.72%, 12.69% and 53.25%, respectively. Finally, the decomposition process of RB5 was proposed by the mass spectrometry results. The electric current promotes cobalt ion cycling and PDS activation through electron transfer, and induces Co(II) to promote the activation of PDS, which is the main mechanism of E-Co(II)-PDS system to achieve the robust degradation ability of RB5.


Asunto(s)
Sulfatos/química , Contaminantes Químicos del Agua , Purificación del Agua , Catálisis , Cobalto , Oxidación-Reducción , Agua
17.
Chemosphere ; 300: 134574, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-35427663

RESUMEN

Diclofenac (DCF), as a typical representative of PPCPs, has potential ecotoxicity to the water environment. In this study, ultrasound (US) enhanced ferrous sulfide (FeS)-activated persulfate (PDS) technology (US/FeS/PDS) was used to degrade DCF. By comparing the degradation effects of US, US/PDS, FeS/PDS and US/FeS/PDS systems on DCF, this study confirmed the synergy and strengthening effects of US. The influences of single-factor experimental conditions on the US/FeS/PDS system were investigated and optimized. The FeS catalysts before and after the reaction were characterized and analyzed by X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS). The heterogeneous reaction proceeded on the surface of FeS, and a small part of FeS2 was formed on FeS surface. During the reaction, the proportion of S2- on the catalyst surface decreased from 51% to 44%. Correspondingly, the proportion of Sx2- increased from 21% to 26%. It indicated that S2- was oxidized into Sx2- in the reaction, and the loss electrons of S2- caused the reduction of Fe3+ to Fe2+on the FeS surface, which promoted the cycle between Fe2+ and Fe3+ in turn. Furthermore, SO4- and ‧OH were the main active free radicals, of which the contribution rate of ‧OH was about 34.4%, while that of SO4- was approximately 52.2%. In US/FeS/PDS, the introduction of US could promote the dissolution of iron on the FeS surface. US contributed to the formation of a redox power motor between S2-Sx2- and Fe2+-Fe3+, which continuously decomposed PDS to generate sufficient active SO4- and ‧OH radicals, thereby efficiently and continuously degrading DCF. Finally, the related mechanism of DCF degradation by US/FeS/PDS was summarized. Overall, US/FeS/PDS can not only efficiently degrade and remove DCF, but also has potential application value in organic pollution removal and wastewater purification.


Asunto(s)
Diclofenaco , Contaminantes Químicos del Agua , Diclofenaco/química , Compuestos Ferrosos , Oxidación-Reducción , Ultrasonido , Contaminantes Químicos del Agua/análisis
18.
Chemosphere ; 296: 134033, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35183578

RESUMEN

The adsorption performances of adsorbents to dyes are hard to maintain in a wide pH range because most of the reactions are pH-dependent, developing a cost-effective strategy to break the pH-limitation is significant. In this study, an amphoteric self-floating adsorbent (Am-SA) was synthesized by hollow silica microsphere surface modification, which was useful to capture anionic acid orange 7 (AO7) and cationic crystal violet (CV) dyes, but the adsorption performances were also greatly affected by pH. Fortunately, a co-precipitation phenomenon was noticed when the AO7 and CV solutions were mixed with a 1:1 molecule ratio. The precise structures of AO7 and CV molecules were constructed and the AO7-CV-H2O mixed system was structured by Materials Studio. Besides, this system was involved in a dynamic simulation to reveal the mechanism of the co-precipitation phenomenon. The simulation results showed H2O molecules dispersed out of the system via thermal motions within 30 ps, but the AO7 and CV molecules aggregated to each other via electrostatic attractions. The energy calculations also demonstrated the electrostatic attraction between AO7 and CV is the dominant factor that induced the aggregation. The aggregation phenomena were also observed in various mixed cationic-anionic dyes systems. The removals of dyes significantly improved in a wide pH range in the mixed systems as the captures of the aggregated dye clusters were much easier than that of independent dye molecules, and both co-precipitation and adsorption contributed to it. Proper utilization of the aggregation behaviors between dyes can be regarded as a prospective strategy in cost-effective treatments.


Asunto(s)
Colorantes , Contaminantes Químicos del Agua , Adsorción , Aniones , Colorantes/química , Violeta de Genciana , Estudios Prospectivos , Contaminantes Químicos del Agua/análisis
19.
J Hazard Mater ; 423(Pt A): 126917, 2022 02 05.
Artículo en Inglés | MEDLINE | ID: mdl-34464865

RESUMEN

The ubiquitous present antibiotics in aquatic environment is attracting increasing concern due to the dual problems of bioaccumulation toxicity and antibiotic resistance. In this study, a low-cost chitin-biocalcium (CC) composite was developed by a facile alkali activation process from shell waste for typical antibiotics ciprofloxacin (CIP) removal. Response surface methodology (RSM) was utilized to optimize synthesis methodology. The optimized CC products featured superior CIP removal capacity of 2432 mg/g at 25 °C (adsorption combined with flocculation), rapid adsorption kinetics, high removal efficiency (95.58%) and wide pH adaptability (under pH range 4.0-10.0). The functional groups in chitin and high content of biocalcium (Ca2+) endowed CC abundant active sites. The kinetic experimental data was fitted well by pseudo-second-order and intraparticle diffusion model at different concentrations, revealing the removal was controlled by chemisorption and mass transport step. From the macroscopic aspect, flocs were produced with the increase of CIP concentration during the reaction, adsorption combined with flocculation were related to the CIP removal. From the microcosmic aspect, the superior removal performance was attributed to cation bridging, cation complexation among biocalcium-CIP and hydrogen bond between functional groups of chitin and CIP.


Asunto(s)
Ciprofloxacina , Contaminantes Químicos del Agua , Adsorción , Antibacterianos , Quitina , Ciprofloxacina/análisis , Floculación , Concentración de Iones de Hidrógeno , Cinética , Contaminantes Químicos del Agua/análisis
20.
Chemosphere ; 289: 133260, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34906524

RESUMEN

A novel chelating flocculant with branched architectures, polyacrylamide grafted maleoyl chitosan-mercaptoacetic acid (PAM-g-M(CS-MA)), was successfully fabricated using maleic anhydride as the "bridge" between chitosan and polyacrylamide. The functional groups and structural characteristic information of copolymers were obtained via characterization analysis. Flocculation performance was systematically investigated via purifying a series of simulated wastewater containing Cu or Cd. The properties of the flocs were studied to give in-depth evidences for the role of chelation groups and branched architectures in flocculation. Results indicated that PAM-g-M(CS-MA) showed excellent flocculation capacity for heavy metals in high concentrations and was superior to other chelating flocculants. The maximum flocculation efficiency of Cu (93.90%) and Cd (92.47%) was achieved by PAM-g-M(CS-MA) at pH 7, dosage of 100 mg L-1 and stirring speed of 90 rpm. The flocculation mechanisms of PAM-g-M(CS-MA) were deeply explored through the analyses of floc properties. The strong synergistic chelation of mercapto, carboxyl, amide and hydroxyl groups predominated for the capturing of heavy metals; and the branched architectures facilitated the formation of large and stable flocs via adsorption and bridging-furl effect. This study provided a solid foundation for the fabrication of flocculants for heavy metal wastewater treatment.


Asunto(s)
Metales Pesados , Purificación del Agua , Quelantes , Floculación , Aguas Residuales
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