CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Wei Sun,Mushan Xie,Bo Shi,Zhixuan Zhu,Jian Zhang,Ying Wang,Jing Bian,Haibo Wang,Chun Zhao
The selective and simultaneous removal of antibiotics (ABs), antibiotic-resistant bacteria (ARBs), and antibiotic resistance genes (ARGs) from complex water matrices is crucial but remains challenging. Herein, relatively pure nonradical oxidation systems of singlet oxygen ( 1 O 2 ) and reactive trivalent manganese (Mn( III ) aq ) were established through electrofiltration-activated peroxymonosulfate and permanganate processes, respectively. Both systems simultaneously removed ABs, ARBs, and > 99 % of 20 selected ARGs within 15 min, while the addition of anions and nature organic matter slightly inhibited ARB inactivation. A multiperspective investigation confirmed that 1 O 2 demonstrated superior efficacy in ARB inactivation and protein damage compared to Mn( III ) aq , whereas Mn( III ) aq destroyed the ARB cell membrane, induced oxidative stress, and damaged almost all ARGs more rapidly than 1 O 2 . In particular, 1 O 2 exhibited selectivity toward four ARGs, which was attributed to a positive dependence on the 5′-GG-3′ doublet content. Moreover, 1 O 2 and Mn( III ) aq significantly reduced the risks of ARB regrowth and horizontal gene transfer of ARGs while providing resilience in real water matrices with improved energy-effectiveness. The findings of this study offer new insights into nonradical reactive species dominated advanced oxidation processes for controlling antibiotic resistance in real water.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Wei Ding,Huaili Zheng,Yongjun Sun,Zhiwei Zhao,Xinyu Zheng,Yuyang Wu,Weilong Xiao
As(III) oxidation to As(V) is deemed necessary for better arsenic removal, and separation is still the optimal approach for water remediation from As(III). Herein, sulfite (SIV) was adopted to activate MnFe 2 O 4 for simultaneous oxidation and adsorption of As(III) in neutral water. The As(III) removal was more efficient than a peroxidation of As(III) followed by adsorption. The adsorption capacity of MnFe 2 O 4 /S(IV) for As(III) (26.257 mg g −1 ) was much higher than those of MnFe 2 O 4 alone for As(III) (9.491 mg g −1 ) and As(V) (9.142 mg g −1 ). The mechanistic study corroborated that intermediate Mn(III) was the dominant oxidant responsible for rapid oxidation of As(III), and the dual roles of S(IV) as a complexing ligand and a precursor of oxysulfur radicals accelerated the redox cycle of Mn(II)/Mn(III). Moreover, S(IV) enhanced arsenic adsorption by driving more production of monodentate complexes. As(III) can be effectively removed over a wide range of temperatures (283.15–313.15 K) and pH (3–10) with the optimal pH of 7. The effect of coexisting ions and reusability of MnFe 2 O 4 were also investigated. Especially, the superior performance of MnFe 2 O 4 /S(IV) for As(III) removal in various water matrixes may help develop new removal technologies based on active Mn(III) for the water decontamination from As(III).
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Guiyuan Cai,Yu Tian,Lipin Li,Wenxuan Zhang,Rui Huang,Jun Zhang,Qinyu Wang,Hua Xu,Yifeng Zhang
The activation of sulfite [S(IV)] by transition metals, a new generation of advanced oxidation processes, has been widely studied for water purification. However, the application of this process to oxidize and remove arsenite [As(III)] from water through Fe-based S(IV) activation and the associated mechanisms are not fully understood. In particular, rapid removal of As(III) and secondary metal contamination have presented challenges. Herein, we develop a novel sea urchin-like magnetic Fe-Mn bimetallic oxides (FeMnO)-activated S(IV) process to address these issues. Under neutral pH, the FeMnO/S(IV) system achieved a 99.2 % removal of As(III) within only 10 min with residual arsenic concentration below 10 µg/L, and the removed As(III) was fully oxidized to arsenate [As(V)]. Additionally, FeMnO was recyclable and capable of treating actual arsenic-contaminated water. Furthermore, the oxidation mechanism of non-radical active trivalent manganese [Mn(III)] was discovered during the reaction between the FeMnO/S(IV) system and As(III). The FeMnO catalyst activated S(IV) to generate oxysulfur radicals (i.e., SO 5 •– , SO 4 •– and SO 3 •– ), but they were not the primary oxidizing species for As(III). Instead, As(III) oxidation was mainly attributed to the active Mn(III) generated by the electron transfer between the FeMnO catalyst and SO 5 •– radicals. The discovery of active Mn(III) species in this work may provide a new avenue for developing novel Fe-Mn-type adsorbents to purify arsenic-contaminated water.
研究领域:
环境科学
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水处理技术
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化学工程
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Song Gao,Xinghao Wang,Xinhao Wang,Xiru Chen,Sijia Liang,Ziyan Zhou,Shuxia Xu,Yanfen Fang,Juan Gao,Cheng Gu
Aqueous trivalent manganese [Mn(III)], an important reactive intermediate, is ubiquitous in natural surface water containing humic acid (HA). However, the effect of low-molecular-weight organic acids (LMWOAs) on the formation, stability and reactivity of Mn(III) intermediate is still unknown. In this study, six LMWOAs, including oxalic acid (Oxa), salicylic acid (Sal), catechol (Cat), caffeic acid (Caf), gallic acid (Gal) and ethylene diamine tetraacetic acid (EDTA), were selected to investigate the effects of LMWOAs on the degradation of BPA induced by in situ formed Mn(III)-L in the HA/Mn(II) system under light irradiation. The chromophoric constituents of HA could absorb light radiation and generate superoxide radical to promote the oxidation of Mn(II) to form Mn(III), which was further involved in transformation of BPA. Our results implied that different LMWOAs did significantly impact on Mn(III) production and its degradation of BPA due to their different functional group. EDTA, Oxa and Sal extensively increased the Mn(III) concentration from 50 to 100 μM compared to the system without LMWOAs, following the order of EDTA > Oxa > Sal, and also enhanced the degradation of BPA with the similar patterns. In contrast, Cat, Caf and Gal had an inhibitory effect on the formation of Mn(III), which is likely because they consumed the superoxide radicals generated from irradiated HA, resulting in the inhibition of Mn(II) oxidation and further BPA removal. The product identification and theoretical calculation indicated that a single electron transfer process occurred between Mn(III)-L and BPA, forming BPA radicals and subsequent self-coupling products. Our results demonstrated that the LMWOAs with different structures could alter the cycling process of Mn via complexation and redox reactions, which would provide new implications for the removal of organic pollutants in surface water.
研究领域:
环境科学
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化学
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PubMed
高影响因子
Small
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2024
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IF 13
Lili Xu,Jianli Nan,Songxue Han,Zhixuan Yu,Shuangli Wu,Youxing Fang,Shaojun Dong
In nature, active Mn 3+ –ligand complexes produced by laccase catalyzed oxidation can act as the low-molecular mass, diffusible redox mediators to oxidize the phenolic substrates overcoming the limitations of natural enzymes. Learning from the metal–ligand coordination of natural functional units, high-valence Mn metal–organic framework (Mn MOF) is constructed to simulate the catalysis in natural mediator system. Benefiting from the characteristics of nanoscale size, rich metal coordination unsaturated sites, and mixed valence state dominated by Mn(III), Nano Mn(III)-TP exhibits superior laccase-mimicking activity, whose V max (maximal reaction rate) is much higher than that of natural laccase. Referring to natural systems, relevant free radical experiments prove that the material induces the production of active oxygen species with the assistance of carboxylic acid, and active oxygen species further oxidize phenolic substrates. Based on its robust performances, the primary oxidative degradation of an emerging pollutant triclosan (TCS) is creatively applied, an important antiasthmatic medicine terbutaline sulfate (TBT) detection, and the synthesis of non-toxic and black near-natural dyes for dyeing. By simulating the essential mediators of natural enzymatic catalysis, an Mn MOF-based material that demonstrates multiple novel applications is successfully developed, which introduces a new reliable strategy for achieving versatile nature-mimicking catalysis.
研究领域:
催化
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材料科学
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环境化学
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分析化学
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有机合成
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Qiaozhi Zhang,Yang Cao,Zibo Xu,Hanwu Lei,Xiaoguang Duan,James H. Clark,Daniel C. W. Tsang
Production of glycolic acid from renewable resources is a significant challenge considering its extensive market and the depletion of fossil resources. This study accomplished sustainable glycolic acid production from biomass-derived saccharides using a microwave-assisted aerobic oxidation system. Various Mn-biochar catalysts were synthesized using different precursors (MnCl2 and KMnO4) and synthesis temperatures (400–850 °C). Glycolic acid yield from glucose could reach 62.8 Cmol % within 20 min at 180 °C over MnBC-VII-700 (i.e., catalyst derived from Mn(VII) precursor and synthesized at 700 °C). Mn(III) was identified as the catalytically active state by correlation with the catalytic performance. Biochar support is vital for reactant adsorption, electron transfer, and microwave absorption. Transformation from glucose to glycolic acid would experience retro-aldol and oxidation reactions, while oxidation-hydrolysis of the glycosidic bond could be achieved for one-pot oligosaccharide conversion. The yields of glycolic acid reached 43.1, 29.2, and 33.3 Cmol % within 30 min, when the substrates were cellobiose, maltose, and maltotriose, respectively. This study developed a low-cost Mn-biochar catalyst for biomass valorization. The study presents valuable mechanistic insights that can serve as a critical reference for the sustainable production of chemical building blocks in heterogeneous catalysis.
研究领域:
化学工程
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可持续化学
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催化
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可再生能源
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Zhimin Gong,Gaobo Wang,Huanhuan Shi,Shuai Shao,Mengjie Wang,Kun Lu,Shixiang Gao
Catalyzed oxidative coupling reactions mediated by enzyme have been proposed as an effective remediation strategy to remove micropollutants, however, little is known about how the Mn(II) redox cycling affects the horseradish peroxidase (HRP)-mediated reactions in wastewater treatment . Here, we explored the removal of two pharmaceuticals and personal care products (PPCPs), methylparaben (MeP) and acetaminophen (AAP), in HRP-mediated reaction system with dissolved Mn (II). It was found that the conversion rate of AAP was about 284 times higher than that of MeP, and Mn (II) significantly inhibited HRP-catalyzed MeP removal but had little influence on that of AAP. X-ray photoelectron spectroscopy (XPS) and theoretical calculations demonstrated that HRP converted Mn(II) into Mn(III), and then generated MnO 2 colloid, which inhibited the removal of the substrates. Moreover, the results of theoretical calculations also showed that the binding energy between HRP and Mn was 27.68 kcal/mol, which was higher than that of MeP (25.24 kcal/mol) and lower than that of AAP (30.19 kcal/mol). Therefore, when MeP and Mn (II) coexisted in the reaction system, HRP preferentially reacted with Mn(II), which explained the different impacts of Mn (II) on the removal of MeP and AAP. Additionally, Mn (II) significantly altered the product distribution by decreasing the amount of polymerization products. Overall, our work here revealed the roles of Mn (II) in the removal of MeP and AAP mediated by HRP, having strong implications for an accurate assessment of the influence of Mn(II) redox cycling on the removal of PPCPs in wastewater treatment.
研究领域:
环境科学
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生物化学
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Junlei Zhang,Wei Zhao,Shanshan Wu,Renli Yin,Mingshan Zhu
Advanced oxidation processes (AOPs) based on heterogeneous catalytic activated peroxymonosulfate (PMS) have been becoming alternatives to conventional wastewater treatment technologies to directly degrade chemical contaminants. To build dual/multi redox cycles of different metal ions may be an effective means for better PMS activation. Herein, this study designed Mn 3 O 4 /CuBi 2 O 4 with dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) to activate PMS for efficiently decomposing and mineralizing diclofenac sodium (DCF). Under optimal reaction conditions, DCF (50 mg/L) was degraded totally within 10 min, and TOC removal rate reached up to 74.3%. The possible mechanism of PMS activation by Mn 3 O 4 /CuBi 2 O 4 was proposed, wherein dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) on Mn 3 O 4 /CuBi 2 O 4 effectively facilitated PMS activation to generate · O 2 − , 1 O 2 , SO 4 · − and · OH, which was responsible for DCF degradation. Moreover, combined with degraded products detected by high resolution liquid chromatography coupled to mass spectrometry and corresponding toxic assessment results, the possible degradation pathways of DCF were proposed and the relative toxicity of degraded products was evaluated. This work may be useful for developing stronger heterogeneous activators of PMS to construct more efficient AOPs for purifying wastewater.
研究领域:
环境科学
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化学工程
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
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IF 7.149
Xinghao Wang,Wenrui Xiang,Siyuan Wang,Jiali Ge,Ruijuan Qu,Zunyao Wang
Soluble manganese(III), stabilized by ligands as Mn(III)-L complexes, are ubiquitous in natural waters and wastewaters and can potentially serve as both the oxidant and reductant in one-electron transfer reactions with organic contaminants. In this study, the oxidative transformations of 14 phenolic endocrine disrupting chemicals (EDCs) by in situ-formed Mn(III)-L complexes, generated from irradiated water containing Mn(II) and humic acid, were investigated. The pseudo-first-order rate constants (kobs, h–1) of these phenols varied from 1.0 × 10–4 to 5.9 × 10–2. A quantitative structure–activity relationship model was developed, which suggests that the electron-donating ability (EHOMO) of phenolic chemicals was the most important molecular characteristic for the Mn(III)-L-mediated oxidative transformation. Phenol transformation was initiated by the generation of a phenoxyl radical through electron transfer to Mn(III)-L. Subsequent self-coupling reactions between phenoxyl radicals resulted in the formation of self-coupling dimers and trimers. With the addition of simple phenol as a cosubstrate, enhanced transformations of these phenolic EDCs were clearly observed, and cross-coupling products of simple phenol and the substrates were also detected. In addition, a reaction activation energy calculation based on the transition-state theory indicated that the cross-coupling reaction was more likely than the self-coupling reaction to occur in the presence of phenol. This work provides new insights into the environmental fate of phenolic compounds.
研究领域:
环境科学
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化学
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生物学
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2018
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IF 6.653
Xinghao Wang,Siyuan Wang,Ruijuan Qu,Jiali Ge,Zunyao Wang,Cheng Gu
Reaction with soluble Mn(II) has been considered as a main decay pathway for superoxide in natural waters, accompanied by an important Mn redox cycling. In this study, the interaction of Mn(II) and humic acid (HA) was investigated in visible light irradiated water. Our results indicate that HA may play a dual role to act as a photosensitizer to produce superoxide anions (O2–) and as a strong ligand to stabilize the Mn(III), forming soluble Mn(III)L species for substrate transformation. Furthermore, the reaction kinetics, products, and mechanisms of chlorophene (CP) and estradiol (E2) mixture in the Mn(II)/HA/visible light reaction systems were assessed. The removal of CP and E2 was enhanced by 24.3% and 13.2%, respectively, in mixture solution at initial concentration of 1.0 μM for each target contaminant, as compared to the case of single-compound degradation. Product identification and density functional theory calculations indicated that cross-coupling reaction of CP and E2 radicals was more likely to occur than the self-coupling reaction in mixture solution. In addition, estrogenic activities of initial reaction solution were also effectively decreased during the transformation process. These findings provide new insights into Mn(III)-mediated reactions to better understand the environmental fate of organic contaminant mixture in waters.
研究领域:
环境化学
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水处理
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高级氧化过程
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污染物降解
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反应机理
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高影响因子
危险品化学品经营许可证（带存储）