JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Yan Xiao,Liangliang Xiong,Yin Xu,Hui Zhang
In recent years, visible light assisted advanced oxidation processes (AOPs) are appealing in the elimination of pollutants. Herein, an innovative and eco-friendly visible light enhanced Fe 3+ -nitrilotriacetic acid system for the activation of peroxydisulfate (Vis/Fe 3+ -NTA/PDS) was proposed for the removal of bisphenol A (BPA). Fe 3+ -NTA could be dissociated through ligand-to-metal charge transfer (LMCT) to realize the generation of Fe 2+ for the continuous activation of PDS to remove BPA. The use of 0.10 mM Fe 3+ , 0.10 mM NTA and 1.00 mM PDS led to 97.5% decay of 0.05 mM BPA and 66.3% of TOC removal in 30 min with the illumination of visible light at initial pH 3.0. The sulfate and hydroxyl radicals were proved to be the dominant species leading to BPA removal by means of radical scavenging experiments, radical probes and electron paramagnetic resonance (EPR) technique. The effects of various operating parameters, natural water constituents as well as different water matrices on BPA abatement were explored. The intermediate products of BPA degradation were identified and a possible transformation pathway was proposed. Briefly, this research provides an attractive strategy for the remediation of refractory wastewater using NTA assisted with visible light in the homogeneous Fe 3+ /PDS system.
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International Journal of Environmental Research and Public Health
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2022
·Vol. 19
·期 15
·9437
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IF 4.614
Qianli Guo,Xianhu Qi,Jian Zhang,Bo Sun
Aqueous complexes of Mn(III) ion with ligands exist in various aquatic systems and many stages of water treatment works, while HSO3−is a common reductant in water treatment. This study discloses that their encounter results in a process that oxidizes organic contaminants rapidly. Pyrophosphate (PP, a nonredox active ligand) was used to prepare the Mn(III) solution. An approximate 71% removal of carbamazepine (CBZ) was achieved by the Mn(III)/HSO3−process at pH 7.0 within 20 s, while negligible CBZ was degraded by Mn(III) or HSO3−alone. The reactive species responsible for pollutant abatement in the Mn(III)/HSO3−process were SO4•−and HO•. The treatment efficiency of the Mn(III)/HSO3−process is highly related to the dosage of HSO3−because HSO3−acted as both the radical scavenger and precursor. The reaction of Mn(III) with HSO3−follows second-order reaction kinetics and the second-order rate constants ranged from 7.5 × 103to 17 M−1s−1under the reaction conditions of this study, suggesting that the Mn(III)/HSO3−process is an effective process for producing SO4•−. The pH and PP:Mn(III) ratio affect the reactivity of Mn(III) towards HSO3−. The water background constituents, such as Cl−and dissolved organic matter, induce considerable loss of the treatment efficiency in different ways.Keywords:Mn(III);bisulfite;advanced oxidation processes;sulfate radical;micropollutant abatement
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Song Wang,Zhe Wang,Jingmei Xu,Qian Liu,Zhiyan Sui,Xinming Du,Yinghe Cui,Yongjiang Yuan,Junjian Yu,Yan Wang,Yifang Chang
A bead-on-string electrospinning strategy is proposed to solve the dilemma of unstable conduction channel while improving the OH − conductivity of anion exchange membranes (AEMs). Here, poly (aryl ether ketone)-based AEMs are synthesized via N-spirocyclic quaternary ammonium modification, and then processed by electrospinning and sparingly soluble techniques. N-spirocyclic cations are induced to orient during electrospinning, as evidenced by the long-range ordered aggregation of ion clusters through EDX . Therefore, the electrospun membrane exhibits significantly higher conductivity (74 mS cm −1 at 80 °C) and alkaline stability, the conductivity remains above 97% after being kept in a solution of 2 mol/L KOH at 80 °C for 720 h. The swelling of the beaded membrane is only 12%, and the tensile strength is about 24.9 MPa. This work provides a simple and effective method to densify nanofiber mats.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2022
·Vol. 119
·期 30
·e2202682119
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IF 12.779
Mingjie Huang,Yu-Sheng Li,Chuan-Qi Zhang,Chao Cui,Qing-Qing Huang,Mengkai Li,Zhimin Qiang,Tao Zhou,Xiaohui Wu,Han-Qing Yu
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.
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Environmental Science-Water Research & Technology
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2022
·Vol. 8
·期 10
·2231-2244
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IF 5.819
Jun Zhao,Jingquan Wang,Erdeng Du,Yijie Ai,Jingjing Liu,Hongguang Guo
The increasing need for water decontamination under high salinity conditions calls for alternative processes with high efficiency and cost-effective performance, of which electrochemical technologies hold continuous attraction. Compared to several studies under chloride background, contaminant degradation in high sulfate concentrations using electrochemical methods has rarely been studied. In this study, a facile and cost-effective TiO2 nanotube (NT) electrode, coated with a PbO2 layer was fabricated to serve as an anode to degrade the selected contaminant under the condition of high sulfate concentration. 100% removal of 0.05 mM 2,4-dichlorophenol (2,4-DCP) was achieved within 50 minutes at a relatively low current density. Degradation of 2,4-DCP followed pseudo-first-order kinetics in the electrochemical system, and the parameter of current density was proved to have the biggest effect on the pollutant removal performance compared to pH and salt concentrations. The mechanism of 2,4-DCP degradation followed the radical and direct electron transfer (DET) pathways. Even though the sulfate radical was generated in water containing high sulfate, the theoretical energy barrier calculated from density functional theory (DFT) simulation indicates the priority of hydroxyl radical on pollutant degradation, and the comparison of reaction energy based on experiments and DFT also suggested that the sulfate radical is more prone to act as a precursor for more hydroxyl radical formation. The degradation performance under various salt conditions was also investigated in this study. High content of chloride in water resulted in extremely fast removal performance, while high content of nitrate in water resulted in the apparent inhibition of pollutant removal. The as-made electrodes exhibited excellent performance for the degradation of different contaminants and reliable stability after rounds of use. This study provides an insight into the application of an electrochemical oxidation system in high salinity wastewater treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zhuoyu Bu,Minhui Hou,Zihao Li,Zhujun Dong,Lusha Zeng,Peng Zhang,Guangyu Wu,Xiang Li,Ying Zhang,Yuwei Pan
Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe 2+ enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe 2+ /PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe 2+ /PMS (B/Fe 2+ /PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that OH and SO 4 − played important role and Fe(IV), 1 O 2 and O 2 − also participated in SMT removal. The addition of boron could enhance the role of OH and SO 4 − in SMT removal in Fe 2+ /PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe 2+ . Possible SMT degradation pathway was proposed. B/Fe 2+ /PMS process could efficiently remove SMT at low Fe 2+ dosage and neutral pH. B/Fe 2+ /PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe 2+ /PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others’ works also demonstrated the present study process was a promising strategy for antibiotics removal.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Honglong Zhang,Zhenyu Shi,Jun Ma,Fuyi Cui,Jing Zhang,Timothy J. Strathmann
In this study, a representative redox mediator, 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO), and its para-substituted derivatives (TEMPOs: 4-hydroxyl-TEMPO, 4-acetylamino-TEMPO, and 4-amino-TEMPO) significantly accelerated the abatement of trace organic contaminants (TrOCs, i.e., bisphenol-A (BPA), phenol, amines, and phenylbutazone) by Mn(VII) over a wide pH range of 4.0–9.0. The addition of substituents at para to the > N–O• moiety significantly influenced the degradation kinetics of TrOCs by changing the reduction potentials of TEMPOs and the corresponding oxoammonium cations (TEMPOs+); a linear relationship was observed between the substituents’ para Hammett sigma constants and the reduction potentials of TEMPOs and TEMPOs+. Pseudo-first-order reaction rate constants (kobs, min–1) of TrOC degradation by Mn(VII)/TEMPOs were also affected by the pKa of the TrOCs. Generally, the highest kobs values for individual TrOCs were observed at pH near the pKa even for TEMPOs+ with relatively pH-invariant reduction potentials. Overall, TrOC abatement kinetics were related to a combination of reactive species (Mn(VII), in situ formed MnO2, and TEMPOs+). For BPA, the relative contributions (R) of reactive species ranked as R(TEMPOs+) > R(Mn(VII)) > R(in situ formed MnO2) at pH 4.0–8.0, whereas R(Mn(VII)) > R(TEMPOs+) at pH 9.0 mainly owing to a change in BPA speciation as the pH approached the pKa1 value for BPA. The results of this study are useful for the development of heterogeneous TEMPO-based redox mediators and future applications of TEMPO-mediated oxidation systems for accelerated abatement of TrOCs in water.
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RESOURCES CONSERVATION AND RECYCLING
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2022
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IF 13.716
Di Zhang,Shaowei Hu,Zhiqin Cao,Hongbin Cao,Yuehong Zhao,He Zhao
To address aggravating environmental and energy problems, the harmless treatment and resource utilization of waste has become an inevitable choice. In this study, we report a highly efficient and low-carbon reuse approach of coagulation sludge waste based catalysts for electro-Fenton(EF) process to treat wastewater. The results showed that the relative amount of iron element in flocs increase gradually along with the growth in coagulant dosage, the main composition of floc is iron-HA complex and the interaction force acting between them was weak complexation. According to evaluation by electrochemical characterization, the selectivity of sludge electrodes for hydrogen peroxide in Oxygen Reduction Reaction (ORR) process was more than 40%. Without add additional Fe 2+ , the as-prepared cathode material is able to achieves 98.7% bisphenol A (BPA) pollutant removal from wastewater within 130 min treatment due to its highly active two-electron reduction of oxygen (O 2 ). Based on life cycle assessment (LCA) results, compared to traditional sludge disposal, the raw sludge used for EF could reduce fossil resource consumption by 73.7% and carbon emissions by more than 97.1%. The coagulation sludge applied in the field of EF in this paper proposes a novel and reliable way of collaborative treatment of sludge and sewage pollutants, and has certain guiding significance in environmental treatment and sludge recycling.
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CHEMOSPHERE
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2022
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IF 8.943
Xuechun Yang,Xiaoyi Zhang,Xinwei Chen,Xiaoying Gao,Yunjia Liu,Jinlan Weng,Shenghong Yang,Tian Gui,Xiangshu Chen,Rusong Zhao,Jian Liu
Achieving both rapid adsorption rate and high adsorption capacity for bisphenol micropollutants from aquatic systems is critical for efficient adsorbents in water remediation . Here, we elaborately prepared three nitrogen-rich triazine-based porous polymers (NTPs) with similar geometric configurations and nitrogen contents (41.70–44.18 wt%) while tunable BET surface areas and micropore volumes in the range of 454.7–536.3 m 2 g −1 and 0.20–0.84 cm 3 g −1 , respectively. It was systematically revealed that the synergy of hydrogen bonding, π−π electron-donor-acceptor interaction, and micropore preservation promoted the rapid (within 5 min) and high capacity adsorption of bisphenols by NTPs. Particularly, microporous-dominated NTPs-3 with the highest micro-pore volume (0.84 cm 3 g −1 ) displays remarkable adsorption capacity towards bisphenol A as evidenced by the adsorption capacity of 182.23 mg g −1 . A simple column filter constructed by NTPs-3 also expressed good dynamic adsorption and regeneration capacity. This work provided new insight into the rational design and engineering of nitrogen-rich porous polymers for the remediation of micropollutant wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qikai Shentu,Zenglong Wu,Wenkai Song,Shiyuan Pan,Zhenyang Zhou,Weiyang Lv,Changsheng Song,Yuyuan Yao
Developing metal-free catalysts for persulfate-mediated oxidation process has been extensively pursued in environmental remediation, yet the activity of these catalysts is typically low and the mechanism is ambiguous. Herein, a facile one-step pyrolysis method was employed to synthesize the carbon doped boron nitride (C-BN) derived from polydopamine coated BN nanosheets. The C-BN could readily activate peroxymonosulfate (PMS) with the activation energy as low as 14.95 kJ/mol, giving rise to admirable performance for bisphenol A removal even at 0 ℃, which was superior to most reported metal-free catalysts. The combined experimental and density functional theory (DFT) analyses pointed out that the remarkable performance of C-BN originated from the B-N-C moieties, which could induce the electron transfer from catalyst to PMS to promote the fast generation of superoxide radicals (O 2 •− ) as the dominant reactive species. These findings take a step toward exploring the highly efficient metal-free catalysts for realistic applications.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Ruiting Sun,Fuwei Lu,Chunmei Yu,Yanan Yang,Lizhen Qiao,Anmin Liu
In the present work, a type of biochar materials derived from carbonizing peanut shells were obtained and employed as the adsorbents of pipette-tip solid-phase extraction (PT-SPE) for the enrichment and determination of six endocrine-disrupting phenols (EDPs) in combination with high-performance liquid chromatography equipped with ultraviolet detector (HPLC-UV). Abundant aliphatic and aromatic carbon structures and functional groups from polar heteroatoms (N, O, S) were distributed in the low-cost and eco-friendly peanut shells-derived biochar materials and were favorable for the enrichment of target EDPs. Moreover, the theoretical calculation based on density functional theory (DFT) proved that the effective enrichment of EDPs in aqueous samples benefited from the effective adsorption on the peanut shells-derived biochar materials. The experimental factors influencing the extraction efficiency were investigated, including adsorbent amount, aspirating/dispensing cycles, the type of elution solvent and elution times, salt addition, sample solution pH and type and volume of washing solvent. Under the optimal conditions, the proposed PT-SPE method exhibited good linear relationship (R 2 > 0.993) in the range of 0.5–400 µg/L and low limits of detections (LODs) from 0.25 to 2.5 µg/L, as well as good precision and accuracy with relative standard deviations (RSDs) of 0.3%–13.2% and recoveries of 83.5%–117.1%. Finally, the biochars-based miniaturized pretreatment method was employed for the determination of six EDPs in bottled water, milk, tea beverage and disposal plastic bag soaked solution with recoveries from 77.5% to 116.5%.
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ENVIRONMENTAL TECHNOLOGY
·
2022
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IF 3.475
Xujia You,Limei Wu,Deqiang Wang,Zhichao Xue,Mingyu Zhao,Xiaolong Wang,Qingxin Liu,Ning Tang
Due to the good photocatalytic performance, which ensures the decomposition of pollutants under light, g-C3N4 is considered as an ideal photocatalytic material. Montmorillonite has a high adsorption capacity and layered structure, which has positive effects on increasing the specific surface area of g-C3N4 and avoid its polymerization agglomeration. In this paper, montmorillonite was used as carrier for g-C3N4 to obtain a new photocatalytic composite g-C3N4/Mt. Then the morphological and (micro)structural properties were characterized. The well-characterized materials were evaluated for the photocatalytic activity in degradation of methylene blue and Bisphenol A. The effects of the mass fraction of g-C3N4, light irradiation time, and pollutant concentration on the photocatalytic performance of g-C3N4/Mt composites were studied. Under the optimal experimental plan, the rate of photocatalytic degradation can reach to 99.3% within 120 min. Through the MS spectrum, it can be found that methylene blue molecule were catalysed and degraded into many harmless substances with low-molecular weight. Finally, based on the obtained reaction products, the mechanism by which the pollutants are removed was proposed. This study provides a new strategy to improve the photocatalysis ability of g-C3N4, which is of great significance for a sustainable pollution treatment.
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