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Occurrence of bisphenol A in surface and drinking waters and its physicochemical removal technologies

Liping LIANG,Jing ZHANG,Pian FENG,Cong LI,Yuying HUANG,Bingzhi DONG,Lina LI,Xiaohong GUAN

《环境科学与工程前沿（英文）》 2015年 第9卷 第1期   页码 16-38 doi: 10.1007/s11783-014-0697-2

摘要： Bisphenol A (BPA), an endocrine disrupting compound, has caused wide public concerns due to its wide occurrence in environment and harmful effects. BPA has been detected in many surface waters and drinking water with the maximum concentrations up to tens of μg·L . The physicochemical technology options in eliminating BPA can be divided into four categories: oxidation, advanced oxidation, adsorption and membrane filtration. Each removal option has its own limitation and merits in removing BPA. Oxidation and advanced oxidation generally can remove BPA efficiently while they also have some drawbacks, such as high cost, the generation of a variety of transformation products that are even more toxic than the parent compound and difficult to be mineralized. Only few advanced oxidation methods have been reported to be able to mineralize BPA completely. Therefore, it is important not only to identify the major initial transformation products but also to assess their estrogenic activity relative to the parent compounds when oxidation methods are employed to remove BPA. Without formation of harmful by-products, physical separation methods such as activated carbon adsorption and membrane processes are able to remove BPA in water effluents and thus have potential as BPA removal technologies. However, the necessary regeneration of activated carbon and the low BPA removal efficiency when the membrane became saturated may limit the application of activated carbon adsorption and membrane processes for BPA removal. Hybrid processes, e.g. combining adsorption and biologic process or combining membrane and oxidation process, which can achieve simultaneous physical separation and degradation of BPA, will be highly preferred in future.

关键词： Bisphenol A (BPA)     occurrence     conventional oxidation     advanced oxidation     adsorption     membrane filtration    

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Enhancement of the electrocatalytic oxidation of antibiotic wastewater over the conductive black carbon-PbO

Xiangyu Wang, Yu Xie, Guizhen Yang, Jiming Hao, Jun Ma, Ping Ning

《环境科学与工程前沿（英文）》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1201-9

摘要： • A novel conductive carbon black modified lead dioxide electrode is synthesized. • The modified PbO2 electrode exhibits enhanced electrochemical performances. • BBD method could predict optimal experiment conditions accurately and reliably. • The modified electrode possesses outstanding reusability and safety. The secondary pollution caused by modification of an electrode due to doping of harmful materials has long been a big concern. In this study, an environmentally friendly material, conductive carbon black, was adopted for modification of lead dioxide electrode (PbO2). It was observed that the as-prepared conductive carbon black modified electrode (C-PbO2) exhibited an enhanced electrocatalytical performance and more stable structure than a pristine PbO2 electrode, and the removal efficiency of metronidazole (MNZ) and COD by a 1.0% C-PbO2 electrode at optimal conditions was increased by 24.66% and 7.01%, respectively. Results revealed that the electrochemical degradation of MNZ wastewater followed pseudo-first-order kinetics. This intimates that the presence of conductive carbon black could improve the current efficiency, promote the generation of hydroxyl radicals, and accelerate the removal of MNZ through oxidation. In addition, MNZ degradation pathways through a C-PbO2 electrode were proposed based on the identified intermediates. To promote the electrode to treat antibiotic wastewater, optimal experimental conditions were predicted through the Box-Behnken design (BBD) method. The results of this study suggest that a C-PbO2 electrode may represent a promising functional material to pretreat antibiotic wastewaters.

关键词： Conductive carbon black     PbO2 electrode     Metronidazole     Electrochemical oxidation     Box-Behnken design-response surface method    

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Catalytic oxidation of CO over Pt/Fe

Zihao Li, Yang Geng, Lei Ma, Xiaoyin Chen, Junhua Li, Huazhen Chang, Johannes W. Schwank

《环境科学与工程前沿（英文）》 2020年 第14卷 第4期 doi: 10.1007/s11783-020-1244-y

摘要： Abstract • Strong metal-support interaction exists on Pt/Fe3O4 catalysts. • Pt metal particles facilitate the formation of oxygen vacancies on Fe3O4. • Fe3O4 supports enhance the strength of CO adsorption on Pt metal particles. The self-inhibition behavior due to CO poisoning on Pt metal particles strongly impairs the performance of CO oxidation. It is an effective method to use reducible metal oxides for supporting Pt metal particles to avoid self-inhibition and to improve catalytic performance. In this work, we used in situ reductions of chloroplatinic acid on commercial Fe3O4 powder to prepare heterogeneous-structured Pt/Fe3O4 catalysts in the solution of ethylene glycol. The heterogeneous Pt/Fe3O4 catalysts achieved a better catalytic performance of CO oxidation compared with the Fe3O4 powder. The temperatures of 50% and 90% CO conversion were achieved above 260°C and 290°C at Pt/Fe3O4, respectively. However, they are accomplished on Fe3O4 at temperatures higher than 310°C. XRD, XPS, and H2-TPR results confirmed that the metallic Pt atoms have a strong synergistic interaction with the Fe3O4 supports. TGA results and transient DRIFTS results proved that the Pt metal particles facilitate the release of lattice oxygen and the formation of oxygen vacancies on Fe3O4. The combined results of O2-TPD and DRIFTS indicated that the activation step of oxygen molecules at surface oxygen vacancies could potentially be the rate-determining step of the catalytic CO oxidation at Pt/Fe3O4 catalysts. The reaction pathway involves a Pt-assisted Mars-van Krevelen (MvK) mechanism.

关键词： Strong metal-support interaction (SMSI)     Surface oxygen vacancy     Lattice oxygen     Magnetite     Platinum metals    

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A perspective on the promoting effect of Ir and Au on Pd toward the ethanol oxidation reaction in alkaline

S. Y. SHEN, Y. G. GUO, G. H. WEI, L. X. LUO, F. LI, J. L. ZHANG

《能源前沿（英文）》 2018年 第12卷 第4期   页码 501-508 doi: 10.1007/s11708-018-0586-7

摘要： There remain great challenges in developing highly efficient electrocatalysts with both high activity and good stability for the ethanol oxidation reaction in alkaline media. Herein, two architectures of tri-metallic PdIrAu/C electrocatalysts are designed and the promoting effect of Au and Ir on Pd toward the ethanol oxidation reaction (EOR) in alkaline media is investigated in detail. On the one hand, the tri-metallic Pd Au Ir/C electrocatalyst with a solid solution alloy architecture is less active relative to Pd Ir/C and Pd/C while the stabilizing effect of Au leads to both a higher activity and a lower degradation percentage after 3000 cycles of the accelerated degradation test (ADT) on Pd Au Ir/C than those on Pd Ir/C. On the other hand, the tri-metallic Pd Ir@(1/3Au)/C electrocatalyst with a near surface alloy architecture delivers a much higher activity with an improvement up to 50.4% compared to Pd Ir/C. It is speculated that for the tri-metallic Pd Ir@(1/3Au)/C electrocatalyst, certain Au atoms are well designed on surfaces to introduce an electronic modification, thus leading to an anti-poisoning effect and improving the EOR activity.

关键词： fuel cells     catalysts     ethanol oxidation     alkaline media     solid solution alloy     near surface alloy    

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Adsorption of toluene, ethylbenzene and xylene isomers on multi-walled carbon nanotubes oxidized by different concentration of NaOCl

Fei YU, Jie MA, Yanqing WU

《环境科学与工程前沿（英文）》 2012年 第6卷 第3期   页码 320-329 doi: 10.1007/s11783-011-0340-4

摘要： Multi-walled carbon nanotubes (MWCNTs) were fabricated and oxidized by different concentrations of sodium hypochlorite (NaOCl) solutions. The untreated MWCNTs and modified MWCNTs were employed as adsorbents to study their characterizations and adsorption performance of toluene, ethylbenzene and xylene isomers (TEX) in an aqueous solution. The physicochemical properties of MWCNTs were greatly affected after oxidation, which influences TEX adsorption capacity. The 3% NaOCl-oxidized MWCNTs shows the greatest enhancement in TEX adsorption, followed by the 30% NaOCl. More interestingly, the 15% NaOCl-oxidized MWCNTs has lower adsorption capacities than untreated MWCNTs. The adsorption mechanism of TEX on treated MWCNTs is attributed to the combined action of hydrophobic interaction, π-π bonding interaction between the aromatic ring of TEX and the oxygen-containing functional groups of MWCNTs and electrostatic interaction. 3% NaOCl solution could not only introduce much oxygen-containing functional groups on MWCNTs, but also lead to less damage for the pore structure. This suggests that the CNTs-3% NaOCl is efficient adsorbent for TEX and that they may possess good potential for TEX removal in wastewater treatment.

关键词： adsorption     toluene     ethylbenzene and xylene isomers (TEX)     multi-walled carbon nanotube     surface oxidation    

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Phenolic compounds removal by wet air oxidation based processes

Linbi Zhou, Hongbin Cao, Claude Descorme, Yongbing Xie

《环境科学与工程前沿（英文）》 2018年 第12卷 第1期 doi: 10.1007/s11783-017-0970-2

摘要： Wet air oxidation (WAO) and catalytic wet air oxidation (CWAO) are efficient processes to degrade organic pollutants in water. In this paper, we especially reviewed the WAO and CWAO processes for phenolic compounds degradation. It provides a comprehensive introduction to the CWAO processes that could be beneficial to the scientists entering this field of research. The influence of different reaction parameters, such as temperature, oxygen pressure, pH, stirring speed are analyzed in detail; Homogenous catalysts and heterogeneous catalysts including carbon materials, transitional metal oxides and noble metals are extensively discussed, among which Cu based catalysts and Ru catalysts were shown to be the most active. Three different kinds of the reactor implemented for the CWAO (autoclave, packed bed and membrane reactors) are illustrated and compared. To enhance the degradation efficiency and reduce the cost of the CWAO process, biological degradation can be combined to develop an integrated technology.

关键词： Wet air oxidation     Catalytic wet air oxidation     Phenolic compounds     Heterogeneous catalysts     Mechanism    

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β-Cyclodextrin promoted oxidation of primary amines to nitriles in water

Dongpo SHI, Hongbing JI, Zhong LI

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 196-200 doi: 10.1007/s11705-009-0051-6

摘要： A facile, efficient and substrate-selective oxidation of the primary amines with NaClO as oxidant catalyzed by cyclodextrin ( CD) has been developed in water for the first time, and the behavior of cyclodextrin that catalyzed the primary amines to nitriles in water was investigated. It was found that the primary amines which could form host-guest complexes with cyclodextrin were oxidized to nitriles with excellent yields at ambient temperature. The results show that cyclodextrin worked not only as a solubilizing agent but also as a catalyst in these reactions.

关键词： substrate-selective     amines oxidation     β-cyclodextrin    

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Solvent-free mechanochemical mild oxidation method to enhance adsorption properties of chitosan

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1416-4

摘要：

• Solvent-free chitosan oxidation is obtained by rapid mechanochemical reaction.

关键词： Chitosan     High energy ball milling     Mechanochemistry     Oxidation    

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Plasma-assisted oxidation of benzoic acid

Anna Khlyustova, Nikolay Sirotkin

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 513-521 doi: 10.1007/s11705-019-1825-0

摘要： Plasma-assisted oxidation of organic compounds is one of the developing technologies for wastewater treatment. Plasmas effectively accelerate degradation processes due to plasma generated reactive species and ultra-violet radiation. Oxidation of benzoic acid in aqueous solutions by the atmospheric pressure glow discharge and underwater diaphragm discharge was studied and monitored by fluorescence and spectrophotometric methods. Discharge type and solution pH affect the formation rates of mono- and dihydroxybenzoic acids. Dihydroxyl derivatives were formed only by glow discharge action. The yields of hydroxyl radical were estimated on the kinetics data for the hydroxylation of benzoic acid. The steps of the hydroxylation processes and further oxidation were described.

关键词： atmospheric pressure glow discharge     underwater diaphragm discharge     oxidation     benzoic acid     hydroxyl radical    

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Novel coprecipitation–oxidation method for recovering iron from steel waste pickling liquor

Shejiang Liu, Hongyang Yang, Yongkui Yang, Yupeng Guo, Yun Qi

《环境科学与工程前沿（英文）》 2017年 第11卷 第1期 doi: 10.1007/s11783-017-0902-1

摘要： Coprecipitation–oxidation method was developed to recover the iron from wastewater. Fe O nanoparticles were well synthesized from steel waste pickling liquor. Promoters greatly improved the properties of synthesized Fe O nanoparticle. Real-time control of the Fe /Fe molar ratio was achieved by ORP monitoring. Waste pickling liquors (WPLs) containing high concentrations of iron and acid are hazardous waste products from the steel pickling processes. A novel combined coprecipitation–oxidation method for iron recovery by Fe O nanoparticle production from the WPLs was developed in this study. An oxidation–reduction potential monitoring method was developed for real-time control of the Fe /Fe molar ratio. The key coprecipitation–oxidation parameters were determined using the orthogonal experimental design method. The use of promoters greatly improved the Fe O nanoparticle crystallinity, size, magnetization, and dispersion. X-ray diffraction patterns showed that the produced Fe O nanoparticles were single phase. The Fe O nanoparticles were approximately spherical and slightly agglomerated. Vibrating sample magnetometry showed that the Fe O nanoparticles produced from the WPLs had good magnetic properties, with a saturation magnetization of 80.206 emu·g and a remanence of 10.500 emu·g . The results show that this novel coprecipitation–oxidation method has great potential for recycling iron in WPLs.

关键词： Waste pickling liquor     Coprecipitation–oxidation     Fe3O4 nanoparticles     Oxidation–reduction potential     Promoter    

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Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

《环境科学与工程前沿（英文）》 2022年 第16卷 第4期 doi: 10.1007/s11783-021-1476-5

摘要：

• MES was constructed for simultaneous ammonia removal and acetate production.

关键词： Biocathode     Carbon dioxide     Electrochemical oxidation     Graphite anode     Boron-doped diamond    

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Application of permanganate in the oxidation of micropollutants: a mini review

Xiaohong GUAN, Di HE, Jun MA, Guanghao CHEN

《环境科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 405-413 doi: 10.1007/s11783-010-0252-8

摘要： As a green oxidant, permanganate has received considerable attention for the removal of micropollutants in drinking water treatment. To provide a better understanding of the oxidation of organic micropollutants with permanganate, the oxidation kinetics of 32 micropollutants were compiled. The pollutants include algal toxins, endocrine disrupting chemicals (EDCs), and pharmaceuticals. The oxidation kinetics of micropollutants by permanganate were found to be first order with respect to both contaminant and permanganate concentrations from which second-order rate constants ( ″) were obtained. Permanganate oxidized the heterocyclic aromatics with vinyl moiety (i.e., microcystins, carbamazepine, and dichlorvos) by the addition of double bonds. For the polycyclic aromatic hydrocarbons (PAHs) with alkyl groups, permanganate attacked the benzylic C-H through abstraction of hydrogen. The mechanism for the oxidation of phenolic EDCs by permanganate was a single electron transfer and aromatic ring cleavage. The presence of background matrices could enhance the oxidation of some phenolic EDCs by permanganate, including phenol, chlorinated phenols, bisphenol A, and trichlosan. The toxicity of dichlorvos solution increased after permanganate oxidation, and the estrogenic activity of bisphnol A/estrone increased significantly at the beginning of permanganate oxidation. Therefore, the toxicity of degradation products or intermediates should be determined in the permanganate oxidation processes to better evaluate the applicability of permanganate. The influence of background ions on the permanganate oxidation process is far from clear and should be elucidated in the future studies to better predict the performance of permanganate oxidation of micropollutants. Moreover, methods should be employed to catalyze the permanganate oxidation process to achieve better removal of micropollutants.

关键词： pharmaceuticals     endocrine disrupting chemicals (EDCs)     algal toxins     permanganate     oxidation    

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“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 207-212 doi: 10.1007/s11705-009-0240-3

摘要： With the rapid expansion of the global motor vehicle population, the transportation sector has taken up a growing proportion among all the carbon dioxide emission-related sectors. To contribute to solutions of the carbon dioxide-oriented problem in transportation, this paper proposes the “ALL FREE” concept that applies partial oxidation process instead of the conventional complete oxidation to vehicle engines. In such an engine, the fuels are partially oxidized into corresponding chemical products, which, as a result, enable the process to be theoretically free of CO, while the heat output of the partial oxidation could drive the vehicle. On the other hand, the resulting products are of great value, which could decrease or even counteract the cost of fuels in transportation. In this paper, the thermodynamic and kinetic data (e.g., the heat output and heat release rate) of five selected partial oxidation reactions were calculated at length to demonstrate and exemplify the theoretical feasibility of the “ALL FREE” concept. It turned out that the partial oxidation of -butane to maleic anhydride has the most potential to meet the basic requirements of this concept. To sum up, this design concept is of significant application potential for the reduction of CO emissions in the transportation industry, although there remain many technical challenges.

关键词： oxidation process     CO     complete oxidation     ALL FREE     -butane    

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Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst

Longli Bo, Shaoyuan Sun

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 385-392 doi: 10.1007/s11705-018-1738-3

摘要： A novel Cu-Mn-Ce/cordierite honeycomb catalyst was prepared by an incipient wetness method and the catalyst was characterized. The active ingredients were present as various spinel species of Cu, Mn and Ce oxides with different valences and they were unevenly dispersed over the surface of the catalyst. The catalytic oxidation of gaseous toluene was primarily investigated using a fixed bed reactor under microwave heating in the continuous flow mode. Under the optimal conditions of 6.7 wt-% loading of the active component, a bed temperature of 200°C, a flow rate of 0.12 m ·h and an initial concentration of toluene of 1000 mg·m , the removal and mineralization efficiencies of toluene were 98% and 70%, respectively. Thus the use of the microwave effectively improved the oxidation of toluene and this is attributed to dipole polarization and hotspot effects. After four consecutive cycles (a total of 1980 min), the Cu-Mn-Ce/cordierite catalyst still exhibited excellent catalytic activity and structural stability, and the toluene removal was higher than 90%. This work demonstrates the possibility of treating volatile organic compounds in exhaust gases by microwave-assisted catalytic oxidation.

关键词： microwave     catalytic oxidation     toluene     Cu-Mn-Ce/cordierite     mineralization    

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Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1345-7

摘要： Abstract • Electrode fouling is characterized by non-destructive characterization. • Electrode fouling is highly dependent on electrochemical process. • Active chlorine can prevent the formation of polymeric fouling film. Electrode fouling is a problem that commonly occurs during electro-oxidation water purification. This study focused on identifying the fouling behavior of Pt electrode associated with the formation of polymeric layer during electro-oxidation of phenol. The in situ electrochemical measurements and non-destructive observation of the electrode morphology were reported. The results demonstrated that the electrode fouling was highly dependent on thermodynamic process of electrode that was controlled by anode potential. At anode potential lower than 1.0 V vs SHE, the direct electro-oxidation caused the electrode fouling by the formation of polymeric film. The fouling layer decreased the electrochemically active surface area from 8.38 cm2 to 1.57 cm2, indicated by the formation of polymeric film with thickness of 2.3 mm, increase in mass growing at a rate of 3.26 μg/cm2/min. The degree to which the anode was fouled was independent of anion in the electrolyte. In comparison, at anode potential higher than 2.7 V vs SHE, the anions (e.g., chloride) could exert a major influence to the behavior of electrode fouling. The presence of chloride was shown to mitigate the fouling of electrode significantly through preventing the formation of polymeric film by active chlorine (e.g., Cl• and Cl2) produced from anodic oxidation of chloride. Since chloride is the most abundant anionic species existing in both natural and engineered water system, this study not only offers a deep insight into the mechanism of electrode fouling, but also suggests strategies for anti-fouling in the presence of chloride in electro-oxidation process.

关键词： Electro-oxidation     Electrode fouling     Polymeric film     Chloride ions    

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标题 作者 时间 类型 操作

Occurrence of bisphenol A in surface and drinking waters and its physicochemical removal technologies

Liping LIANG,Jing ZHANG,Pian FENG,Cong LI,Yuying HUANG,Bingzhi DONG,Lina LI,Xiaohong GUAN

期刊论文

Enhancement of the electrocatalytic oxidation of antibiotic wastewater over the conductive black carbon-PbO

Xiangyu Wang, Yu Xie, Guizhen Yang, Jiming Hao, Jun Ma, Ping Ning

期刊论文

Catalytic oxidation of CO over Pt/Fe

Zihao Li, Yang Geng, Lei Ma, Xiaoyin Chen, Junhua Li, Huazhen Chang, Johannes W. Schwank

期刊论文

A perspective on the promoting effect of Ir and Au on Pd toward the ethanol oxidation reaction in alkaline

S. Y. SHEN, Y. G. GUO, G. H. WEI, L. X. LUO, F. LI, J. L. ZHANG

期刊论文

Adsorption of toluene, ethylbenzene and xylene isomers on multi-walled carbon nanotubes oxidized by different concentration of NaOCl

Fei YU, Jie MA, Yanqing WU

期刊论文

Phenolic compounds removal by wet air oxidation based processes

Linbi Zhou, Hongbin Cao, Claude Descorme, Yongbing Xie

期刊论文

β-Cyclodextrin promoted oxidation of primary amines to nitriles in water

Dongpo SHI, Hongbing JI, Zhong LI

期刊论文

Solvent-free mechanochemical mild oxidation method to enhance adsorption properties of chitosan

期刊论文

Plasma-assisted oxidation of benzoic acid

Anna Khlyustova, Nikolay Sirotkin

期刊论文

Novel coprecipitation–oxidation method for recovering iron from steel waste pickling liquor

Shejiang Liu, Hongyang Yang, Yongkui Yang, Yupeng Guo, Yun Qi

期刊论文

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

期刊论文

Application of permanganate in the oxidation of micropollutants: a mini review

Xiaohong GUAN, Di HE, Jun MA, Guanghao CHEN

期刊论文

“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

期刊论文

Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst

Longli Bo, Shaoyuan Sun

期刊论文

Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

期刊论文