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Impact factors and pathways of halonitromethanes formation from aspartic acid during LED-UV_(265)/Chlorine disinfection

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Frontiers of Environmental Science & Engineering 2024年第1期18卷 129-144页

作者： Liangwen Zhu Tao Wang Qian Tang Qing Wang Lin Deng Jun Hu Chaoqun Tan Rajendra Prasad Singh Key Laboratory of Concrete and Prestressed Concrete Structures of Ministry of Education School of Civil EngineeringSoutheast UniversityNanjing 211189China College of Environment Zhejiang University of TechnologyHangzhou 310014China

Light emitting diode (LED-UV)/Chlorine disinfection can replace UV/Chlorine disinfection in wastewater treatment plants and water supply plants. Halonitromethanes (HNMs) are a class of novel nitrogenous disinfection by-products, which are characterized by higher cytotoxicity and genotoxicity than regulated disinfection by-products. Herein, the impact factors and pathways of HNMs formation from aspartic acid (ASP) were investigated during LED-UV_(265)/Chlorine disinfection. The results showed that three types of chlorinated-HNMs (Cl-HNMs) were found during LED-UV265/Chlorine disinfection, and their concentrations increased first and then declined as the reaction progressed. Cl-HNMs yields increased with increasing LED-UV_(265) intensity, free Chlorine dosage, and ASP concentration, which declined with increasing pH (6.0–8.0). Meantime, the important impact of the coexisting ions contained in water matrices on HNMs formation from ASP was observed during LED-UV_(265)/Chlorine disinfection. It was found that copper ions (Cu^(2+)) promoted Cl-HNMs formation. Furthermore, when bromide (Br–) appeared during LED-UV265/Chlorine disinfection, nine types of HNMs were detected simultaneously. Moreover, Br– not only converted Cl-HNMs toward brominated (chlorinated)-HNMs and brominated-HNMs but also showed a marked effect on HNMs concentrations and species. Subsequently, the possible pathways of HNMs formation from ASP were proposed during LED-UV_(265)/Chlorine disinfection. At last, it was proved that the formation trends of HNMs obtained in the real waters were similar to those in simulated waters. This work elaborated on the influence factors and pathways of HNMs formation, which is conducive to controlling the HNMs produced during LED-UV_(265)/Chlorine disinfection.

关键词： LED-UV265 Chlorine HNMs Aspartic acid Bromide Copper ions

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The Chlorine evolution reaction promoted by organocatalysts with amide functional groups

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Science China Chemistry 2024年第3期67卷 749-750页

作者： Lan Zhao Liang-Nian He State Key Laboratory and Institute of Elemento-Organic Chemistry College of ChemistryNankai UniversityTianjin 300071China

Since the nineteenth century, the chlor-alkali process entails the electrochemical oxidation of sodium chloride solutions to Cl_(2) by the Chlorine evolution reaction(CER) and the simultaneous production of sodium hyd... 详细信息

关键词： Chlorine hydroxide promoted

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Molten hydroxide for detoxification of Chlorine-containing waste: Unraveling Chlorine retention efficiency and Chlorine salt enrichment

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Journal of Environmental Sciences 2019年第8期31卷 192-202页

作者： Shijin Dai Yilin Zheng Youcai Zhao Yu Chen Dongjie Niu College of Environmental Science and Engineering Tongji University Shanghai Institute of Pollution Control and Ecological Security

Hazardous waste dechlorination reduces the potential of creating dioxins during the incineration process. To investigate the salt effect on waste dechlorination, molten hydroxides with a low melting temperature were utilized for the pre-dechlorination and decomposition of Chlorine-containing organic wastes(COWs) including trichlorobenzene(TCB),perchloroethylene, hexachlorobenzene and chlordane. The results showed that a eutectic mixture of caustic sodium and potassium hydroxides(41 wt.% NaOH and 59 wt.% KOH) led to a low melting point below 300°C and a relatively high Chlorine retention efficiency(CRE) with TCB as a representative COWs. The amounts of hydroxides, reaction time, and temperature all had notable influence on CRE. When the mass ratio of hydroxides to TCB reached 30:1,approximately 98.1% of the TCB was destroyed within 2.5 hr at 300°C with CRE of 71.6%.According to the residue analysis, the shapes of reaction residues were irregular with particles becoming swollen and porous. The benzene ring and C–Cl bonds disappeared, while carboxyl groups formed in the residues. The stripped Chlorine was retained and condensed to form chloride salts, and the relative abundance of the chloride ions associated with the mass of TCB in residues increased from 0 to 75.0% within the 2.5 hr reaction time. The observed concentration of dioxins in residues was 5.6 ngTEQ/kg. A reaction pathway and possible additional reactions that occur in this dechlorination system were proposed. Oxidizing agents may attack TCB and facilitate hydrogenation/dechlorination reactions, making this process a promising and environmentally friendly approach for Chlorine-containing organic waste treatment.

关键词： Molten salt Chlorine-containing organic waste Trichlorobenzene Pesticides Chlorine removal Chlorine salt

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Individual stages of bacterial dichloromethane degradation mapped by carbon and Chlorine stable isotope analysis

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Journal of Environmental Sciences 2019年第4期31卷 147-160页

作者： Maria L.Torgonskaya Anatoly M.Zyakun Yuri A.Trotsenko Kestutis S.Laurinavichius Steffen Kümmel Stéphane Vuilleumier Hans H.Richnow Laboratory of Radioactive Isotopes G.K.Skryabin Institute of Biochemistry and Physiology of MicroorganismsFRC Pushchino Center for Biological ResearchRussian Academy of Sciences Laboratory of Mass Spectrometry G.K.Skryabin Institute of Biochemistry and Physiology of MicroorganismsFRC Pushchino Center for Biological ResearchRussian Academy of Sciences Department of Isotope Biogeochemistry Helmholtz Centre for Environmental Research-UFZ Université de Strasbourg CNRS

The fractionation of carbon and Chlorine stable isotopes of dichloromethane(CH_2Cl_2,DCM)upon dechlorination by cells of the aerobic methylotroph Methylobacterium extorquens DM4 and by purified DCM dehalogenases of the glutathione S-transferase family was analyzed.Isotope effects for individual steps of the multi-stage DCM degradation process,including transfer across the cell wall from the aqueous medium to the cell cytoplasm,dehalogenase binding,and catalytic reaction,were considered.The observed carbon and Chlorine isotope fractionation accompanying DCM consumption by cell supensions and enzymes was mainly determined by the breaking of C\Cl bonds,and not by inflow of DCM into cells.Chlorine isotope effects of DCM dehalogenation were initially masked in high density cultures,presumably due to inverse isotope effects of non-specific DCM oxidation under conditions of oxygen excess.Glutathione cofactor supply remarkably affected the correlation of variations of DCM carbon and Chlorine stable isotopes(Δδ^(13)C/Δδ^(37)Cl),increasing corresponding ratio from 7.2–8.6 to 9.6–10.5 under conditions of glutathione deficiency.This suggests that enzymatic reaction of DCM with glutathione thiolate may involve stepwise breaking and making of bonds with the carbon atom of DCM,unlike the uncatalyzed reaction,which is a one-stage process,as shown by quantum-chemical modeling.

关键词： Dichloromethane(DCM) Microbial degradation Aerobic methylotrophic bacteria Dichloromethane dehalogenase Carbon and Chlorine isotopic fractionation

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Review on fate of Chlorine during thermal processing of solid wastes

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Journal of Environmental Sciences 2019年第4期31卷 13-28页

作者： Peng Lu Qunxing Huang A.C.(Thanos) Bourtsalas Nickolas J.Themelis Yong Chi Jianhua Yan State Key Laboratory of Clean Energy Utilization Zhejiang University Earth Engineering Center Columbia University

Chlorine(Cl) is extensively present in solid wastes, causing significant problems during the thermal conversion of waste to energy or fuels, by combustion, gasification or pyrolysis.This paper introduces the analytical methods for determining the Cl content in solid materials and presents the concentrations of Cl in various types of wastes, as reported in literature. Then, it provides a comprehensive analysis on the Cl emission behavior and Cl species formed during the thermal processing of the inorganic and organic Cl sources. The challenges resulted from the reactions between the formed Cl species and the ferrous metals, the heavy metals and the organic matters are summarized and discussed, e.g., high temperature corrosion, heavy metal evaporation and dioxin formation. The quality degradation of products(oil, char and syngas) by Cl is analyzed. Finally, the available controlling methods of Cl emission, including pre-treatment(water washing, sorting,microwave irradiation and stepwise pyrolysis) and in-furnace(absorbents, co-treatment and catalysts) methods are assessed.

关键词： Chlorine Solid wastes Thermal processing Emission Controlling methods

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Inorganic lead-free cesium copper Chlorine nanocrystal for highly efficient and stable warm white light-emitting diodes

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Photonics Research 2021年第2期9卷 187-192页

作者： SHUANGYI ZHAO QIONGHUA MO WENSI CAI HUAXIN WANG ZHIGANG ZANG Key Laboratory of Optoelectronic Technology&Systems(Ministry of Education) Chongqing UniversityChongqing 400044China

Inorganic cesium lead halide(CsPbX_(3), X=Cl, Br, I) nanocrystals(NCs) attract extensive attention because of their excellent optoelectronic performance. However, the classic CsPbX_(3) NCs suffer from toxicity and instability, which impede their further applications in commercial fields. Here the inorganic lead-free cesium copper Chlorine NCs are synthesized by a facile hot-injection method. The blue-emission 3D CsCu_(2)Cl_(3) and green-emission 0DCs_(3)Cu_(2)Cl_(5) NCs are prepared at 70℃ and 120℃, respectively, suggesting that the reaction temperature may account for the final components. Owing to the self-trapped exciton effect, the unique optical properties, such as high photoluminescence(PL) quantum yield, broadband emission, large Stokes shift, and long PL decay time, are demonstrated for both cesium copper Chlorine NCs. Moreover, highly efficient and stable warm white light-emitting diodes are fabricated with CsCu_(2)Cl_(3) and Cs_(3)Cu_(2)Cl_(5) NCs. The study highlights the promising potential for lead-free cesium copper Chlorine nanocrystals in nontoxic solid-state lighting applications.

关键词： method. Chlorine copper

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Chlorine-free emission disposal of spent acid etchant in a three-compartment ceramic membrane reactor

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Chinese Journal of Chemical Engineering 2020年第1期28卷 271-278页

作者： Fanglu Yuan Lele Cui Peipei Ding Wenheng Jing State Key Laboratory of Materials-Oriented Chemical Engineering National Engineering Research Center for Special Separation MembraneCollege of Chemical EngineeringNanjing Tech UniversityNanjing 211800China

Electrochemical technologies for the on-site treatment of spent acid etchant have received great attention due their ease of operation and economic benefits. On the other hand, a large amount of Cl2 is generated during the electrolysis process, which leads to potential environmental risks. In the present work, a novel threecompartment ceramic membrane flow reactor, including a cathode chamber, an anode chamber, and a gas absorption chamber was developed. The three chambers were divided by an Al2O3 ceramic membrane and a breathable hydrophobic anode diffusion electrode(ADE). The Cl2 evolution onset potential of the ADE was increased to 1.19 V from 1.05 V of the graphite felt, effectively inhibiting the Chlorine evolution reaction(CER).The anode-generated Cl2 diffused into the gas absorption chamber through the ADE and was eventually consumed by the H2O2 adsorbent. Cu could be recovered without emitting Chlorine due to the special structure of reactor. The current efficiency of copper precipitation and cathode reduction from Cu2+to Cu+reached 97.7%at a working current of 150 m A. These results indicated that the novel membrane reactor had high potential for application in the copper recovery industry.

关键词： Spent acid etchant Chlorine evolution reaction Anode diffusion electrode Three-compartment reactor Ceramic membrane

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Tuning the Molecular Weight of Chlorine-Substituted Polymer Donors for Small Energy Loss

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Chinese Journal of Chemistry 2021年第6期39卷 1651-1658页

作者： Tingxing Zhao Huan Wang Mingrui Pu Hanjian Lai Hui Chen Yulin Zhu Nan Zheng Feng He Shenzhen Grubbs Institute and Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdong 518055China Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhenGuangdong 518055China Institute of Polymer Optoelectronic Materials and Devices State Key Loborotory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhouGuangdong 510640China Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhenGuangdong 518055China

The molecular weight of polymers plays a major role in their aggregation and miscibility in active layer,which eventually dominate the energy loss and device performance.A series of Chlorine-substituted PBD-CI polymers with controlled molecular weight have been synthesized as templates to discern a relationship between molecular weight and the optical properties,energy levels,morphologies,energy loss and photovoltaic performance.Although it has similar optical and electrochemical properties,when blended with acceptor N3,the low molecular weight polymer PBD-CI_(L) gives the biggest energy loss value,and a PCE of 12.06%.PBD-CI_(H) shows a moderate energy loss,but displays the lowest PCE of 9.00%as a result of excessive aggregation.PBD-CI_(M) with a medium molecular weight gives the smallest energy loss and achieves a PCE of 17.17%,which is among one of the highest values recorded to date for the C卜substituted polymer solar cells.Moreover,the molecular weight mainly affects the nonradiative energy loss(△E_(3)), PBD-CI_(M) also shows the smallest value of 0.252 eV among three polymer donors.These results show the effect of controlling the molecular weight to achieve a small energy loss and provide guidelines which can lead to an understanding of the real photovoltaic performance of new materials.

关键词： Molecular weight Chlorine Miscibility Energy loss Renewable resources

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Effect of photodynamic therapy with(17R,18R)-2-(1-hexyloxyethyl)-2-devinyl Chlorine E6 trisodium salt on pancreatic cancer cells in vitro and in vivo

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World Journal of Gastroenterology 2018年第46期24卷 5246-5258页

作者： Yu-Jie Shen Jia Cao Fang Sun Xiao-Lei Cai Ming-Ming Li Nan-Nan Zheng Chun-Ying Qu Yi Zhang Feng Shen Min Zhou Ying-Wei Chen Lei-Ming Xu Department of Gastroenterology Xinhua Hospital Affiliated to Shanghai Jiao Tong University School of Medicine

AIM To investigate the antitumor effects and underlying mechanisms of(17 R,18 R)-2-(1-hexyloxyethyl)-2-devinyl Chlorine E6 trisodium salt(YLG-1)-induced photodynamic therapy(PDT) on pancreatic cancer in vitro and in vivo.METHODS YLG-1 is a novel photosensitizer extracted from spirulina. Its phototoxicity, cellular uptake and localization, as well as its effect on reactive oxygen species(ROS) production, apoptosis, and expression of apoptosis-associated proteins were detected in vitro. An in vivo imaging system(IVIS), the Lumina K imaging system, and mouse models of subcutaneous Panc-1-bearing tumors were exploited to evaluate the drug delivery pathway and pancreatic cancer growth in vivo.RESULTS YLG-1 was localized to the mitochondria, and the appropriate incubation time was 6 h. Under 650 nm light irradiation, YLG-1-PDT exerted a potent cytotoxic effect on pancreatic cancer cells in vitro, which could be abolished by the ROS scavenger N-acetyl-L-cysteine(NAC). The death mode caused by YLG-1-PDT was apoptosis, accompanied by upregulated Bax and cleaved Caspase-3 and decreased Bcl-2 expression. The results from the IVIS images suggested that the optimal administration route was intratumoral(IT) injection and that the best time to conduct YLG-1-PDT was 2 h post-IT injection. Consistent with the results in vitro, YLG-1-PDT showed great growth inhibition effects on pancreatic cancer cells in a mouse model.CONCLUSION YLG-1 is a potential photosensitizer for pancreatic cancer PDT via IT injection, the mechanisms of which are associated with inducing ROS and promoting apoptosis.

关键词： Photodynamic therapy Pancreatic neoplasm (17R,18R)-2-(1-hexyloxyethyl)-2-devinyl Chlorine E6 trisodium salt Antitumor effect

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A batch microfabrication of a self-cleaning,ultradurable electrochemical sensor employing a BDD film for the online monitoring of free Chlorine in tap water

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Microsystems & Nanoengineering 2022年第2期8卷 85-96页

作者： Jiawen Yin Wanlei Gao Weijian Yu Yihua Guan Zhenyu Wang Qinghui Jin Faculty of Electrical Engineering and Computer Science Ningbo University315211 NingboP.R.China State Key Laboratory of Transducer Technology Shanghai Institute of Microsystem and Information TechnologyChinese Academy of Sciences200050 ShanghaiP.R.China

Free Chlorine is one of the key water quality parameters in tap water.However,a free Chlorine sensor with the characteristics of batch processing,durability,antibiofouling/antiorganic passivation and in situ monitoring of free Chlorine in tap water continues to be a challenging issue.In this paper,a novel silicon-based electrochemical sensor for free Chlorine that can self-clean and be mass produced via microfabrication technique/MEMS(Micro-Electro-Mechanical System)is proposed.A liquid-conjugated Ag/AgCI reference electrode is fabricated,and electrochemically stable BDD/Pt is employed as the working/counter electrode to verify the effectiveness of the as-fabricated sensor for free Chlorine detection.The sensor demonstrates an acceptable limit of detection(0.056 mg/L)and desirable linearity(R^(2)=0.998).Particularly,at a potential of+2.5 V,hydroxyl radicals are generated on the BBD electrode by electrolyzing water,which then remove the organic matter attached to the surface of the sensor though an electrochemical digestion process.The performance of the fouled sensor recovers from 50.2 to 94.1%compared with the initial state after self-cleaning for 30 min.In addition,by employing the MEMS technique,favorable response consistency and high reproducibility(RSDChlorine is observed,ensuring the accuracy of the sensor with any hydrologic parameter.The interesting sensing and selfcleaning behavior of the as-proposed sensor indicate that this study of the mass production of free Chlorine sensors by MEMS is successful in developing a competitive device for the online monitoring of free Chlorine in tap water.

关键词： Chlorine batch electrode

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