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Degradation of iopamidol in the permanganate/sulfite process:Evolution of iodine species and effect on the subsequent formation of disinfection by-products

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Journal of environmental sciences 2024年第1期135卷 345-352页

作者： Yimin Lin Hongyu Dong Yating Zhu Gongming Zhou Junlian Qiao Xiaohong Guan State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Department of environmental science School of Ecological and Environmental SciencesEast China Normal UniversityShanghai 200241China

Permanganate/sulfite(Mn(VII)/S(IV))process is a promising pre-oxidation technology for sequestering the emerging organic contaminants in drinking water treatment plant.Iopamidol(IPM),a representative of iodinated X-ray contrast media,has been widely detected in water sources and has the risk of forming iodinated disinfection byproducts(I-DBPs)in water treatment system.In this study,we investigated the evolution of iodine species during the IPM degradation by the Mn(VII)/S(IV)process and its effect on the subsequent formation of I-DBPs during chlorination at pH 7.0 and 8.0.IPM could be effectively degraded in the Mn(VII)/S(IV)process at environmentally relevant pH(pH 7.0 and 8.0).The results of quenching and competitive oxidation kinetic experiments revealed that SO^(·-)_(4)was the major reactive oxidizing species contributing to the degradation of IPM whereas the contributions of HO·and reactive manganese species were negligible in the Mn(VII)/S(IV)process.I–and IO–3were generated while no HOI was detected during the degradation of IPM in the Mn(VII)/S(IV)process.The effects of IPM oxidation by Mn(VII)/S(IV)on the subsequent formation of chlorinated disinfection by-products(Cl-DBPs)during chlorination were related to the category of Cl-DBPs.The pre-oxidation of IPM by Mn(VII)/S(IV)resulted in the generation of I-DBPs during the disinfection process although no I-DBPs were detected if no pre-oxidation was applied.The finding of this study suggested that attention should be paid to the toxicity of DBPs when water containing iodinated organic contaminants is treated by Mn(VII)/S(IV)process or other pre-oxidation technologies.

关键词： Permanganate/sulfite Iopamidol Sulfate radical Iodinated disinfection byproducts Pre-oxidation

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A novel graphene oxide-carbon nanotubes anchored α-FeOOH hybrid activated persulfate system for enhanced degradation of Orange Ⅱ

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Journal of environmental sciences 2019年第9期31卷 73-84页

作者： Shanshan Su Yuyang Liu Wei He Xianchun Tang Wei Jin Yaping Zhao School of Ecological and Environmental Sciences Shanghai Key Laboratory for Urban Ecological Process and Eco-Restoration East China Normal University Shanghai 200241 China school of environmental science and Engineering and Experimental Teaching Center of Environmental Science and Engineering Tongji University Shanghai 200071 China

Persulfate activation has been applied as one of the efficient advanced oxidation processes(AOPs) to remediate polluted environments. In this study, a novel α-FeOOH anchored by graphene oxide(GO)-carbon nanotubes(CNTs) aerogel(α-FeOOH@GCA) nanocomposite activated persulfate system(α-FeOOH@GCA + K2S2O8) was applied for decolorization of Orange Ⅱ(OⅡ). The decolorization of OⅡ was remarkably enhanced to a level of ~ 99% in this system compared with that of pristine α-FeOOH(~ 44%) or GO-CNTs(~18%). The enhanced catalytic activity of α-FeOOH@GCA was due to the formation of a heterojunction byα-FeOOH and GO-CNTs as confirmed by the presence of Fe–O–C chemical bonds. The degradation intermediates of OⅡ were comprehensively identified. The proposed degradation pathway of OⅡ begins with the destruction of the conjugated structures of OⅡ by the dominant reactive oxygen species, surface-bound SO4·-. The decolorization efficiency of OⅡ by the α-FeOOH@GCA activated persulfate system decreased from the first to third cycle of recycling. Ultraviolet(UV) irradiation or introduction of a small amount of Fe2+ could restore the activation of this system. The results show that the α-FeOOH@GCA persulfate activation system promises to be a highly efficient environmental remediation method for organic pollutants.

关键词： Graphene oxide Goethite Nanocomposite Persulfate activation Dye Wastewater treatment

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Dielectr ic barr ier discharge plasma-assisted modification of g-C_(3)N_(4)/Ag_(2)O/TiO_(2)-NRs composite enhanced photoelectrocatalytic activity

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Journal of environmental sciences 2021年第6期33卷 113-127页

作者： Yupei Long Chenchen Yuan Xiaomin Wang Dongyan Jin Hong Zhou Qiongyin Wang Chenyang Lu Yuqi Chen Yanqing Cong Qi Wang Yi Zhang school of environmental science and Engineering Zhejiang Gongshang UniversityHangzhou310018China ecological environmental science Design and Research Institute of Zhejiang Province Hangzhou310007China

Dielectric barrier discharge(DBD)plasma applied as surface treatment technology was employed for the modification of Ag_(2)O and graphitic carbon nitride(g-C_(3)N_(4))powders.Subsequently,the pretreated powders were sequentially loaded onto TiO_(2)nanorods(TiO_(2)-NRs)via electro-deposition,followed by calcination at N_(2)atmosphere.The results indicated that at the optimal plasma discharge time of 5 min for modification of g-C_(3)N_(4)and Ag_(2)O,photocurrent density of ternary composite was 6 times to bare TiO_(2)-NRs under UV-visible light irradiation.Phenol was degraded by using DBD plasma-modified g-C_(3)N_(4)/Ag_(2)O/TiO_(2)-NRs electrode to analyze the photoelectrocatalytic performance.The removal rate of phenol for g-C_(3)N_(4)-5/Ag_(2)O-5/TiO_(2)-NRs electrode was about 3.07 times to that for TiO_(2)-NRs electrode.During active species scavengers'analysis,superoxide radicals and hydroxyl radicals were the main oxidation active species for pollutants degradation.A possible electron-hole separation and transfer mechanism of ternary composite with high photoelectrocatalytic performance was proposed.

关键词： Degradation mechanism Photoelectrochemical catalysis Plasma treatment Ternary material Z-scheme structure

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environmental arsenic(As)and its potential relationship with endemic disease in southwestern China

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Journal of environmental sciences 2024年第5期139卷 46-59页

作者： Donglin Li Hucai Zhang Fengqin Chang Lizeng Duan Yang Zhang Institute for ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental ScienceYunnan UniversityKunming 650500China Southwest United Graduate school Kunming 650500China

Many cases of an unknown disease exhibiting the clinical features of limb gangrene,blisters,ulceration,and exfoliation have been reported in Daping village(DV)in southwestern China.However,the pathogenesis is unknown and has puzzled doctors for many years.A preliminary study on heavy metals and symptoms indicated that arsenic might pose the greatest threat to the health of local residents.Here,to explore the sources of and factors influencing arsenic enrichment in DV,whose residents exhibit signs of arsenic poisoning,the As contents in soil,water,and plants were systematically measured.The results indicated high As contents in plant and soil samples obtained from the area,and the source of As may be linked to the weathering of black shale rock.Ingestion of soil and consumption of plants were the two main As exposure pathways among children and adults,respectively,and children exhibited a higher health risk than adults.We presume and emphasize that when extreme drought events occur,humans might face unusual risks resulting from exposure to toxic elements and the direct consumption of highly polluted water.Our study provides a new perspective and sheds light on the environmental geochemistry and health links of this disease.

关键词： Endemic disease Arsenic(As) Risk assessment Black shale Climate change

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Surface protection method for the magnetic core using covalent organic framework shells and its application in As(Ⅲ)depth removal from acid wastewater

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Journal of environmental sciences 2022年第5期34卷 1-9页

作者： Wenjun Huang Haomiao Xu Xiaoshuang Liu Longlong Wang Shutang Li Leipeng Ji Zan Qu Naiqiang Yan school of environmental science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China Shanghai Institute of Pollution Control and ecological Security Shanghai 200092China

Fe_(3)O_(4)-based materials are widely used for magnetic separation from wastewater.However,they often suffer from Fe-leaching behavior under acidic conditions,decreasing their ac-tivity and limiting sustainable practical applications.In this study,covalent organic frame-works(COFs)were used as the shell to protect the Fe_(3)O_(4) core,and the Fe_(3)O_(4)@COF core-shell composites were synthesized for As(Ⅲ)removal from acid wastewater.The imine-linked COFs can in situ grow on the surface of the Fe_(3)O_(4) core layer by layer with[COFs/Fe_(3)O_(4)]mol ratio of up to 2∶1.The Fe-leaching behavior was weakened over a wide pH range of 1-13.Moreover,such composites keep their magnetic characteristic,making them favorable for nanomaterial separation.As(Ⅲ)batch adsorption experiments results indicated that,when COFs are used as the shell for the Fe_(3)O_(4) core,a balance between As(Ⅲ)removal efficiencies and the thickness of the COF shell exists.Higher As(Ⅲ)removal efficiencies are obtained when the[COFs/Fe_(3)O_(4)]mol ratios were<1.5∶1,but thicker COF shells were not beneficial for As(Ⅲ)removal.Such composites also exhibited better As(Ⅲ)removal performances in the pH range of 1-7.Over a wide pH range,the zeta potential of Fe_(3)O_(4)@COF core-shell compos-ites becomes more positive,which benefits the capture of negative arsenic ions.In addition,thinner surface COFs were favorable for mass transfer and facilitating the reaction of Fe and As elements.Our study highlights the promise of using COFs in nanomaterial surface protection and achieving As(Ⅲ)depth removal under acidic conditions.

关键词： Arsenic ions Covalent Organic Framework Core-shell structure Surface protectionLayer Thickness

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In-situ generation of gold nanoparticles on MnO_2 nanosheets for the enhanced oxidative degradation of basic dye(Methylene Blue)

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Journal of environmental sciences 2018年第3期30卷 236-245页

作者： Xueqin Bao Zhen Qin Tianshu Zhou Jingjing Deng School of Ecological and Environmental Sciences East China Normal University

In this work,the gold nanoparticles（Au-NPs）were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimize the oxidation of basic dye（Methylene Blue（MB））,including the molar ratio of MnO2to chloroauric acid（HAu Cl4）,the p H of the solution and the effect of initial material.Under the optimal condition,the highest degradation efficiency for MB achieved to 98.9%within 60 min,which was obviously better than commercial MnO2powders（4.3%）and MnO2nanosheets（74.2%）.The enhanced oxidative degradation might attribute to the in-situ generation of ultra-small and highly-dispersed Au-NPs which enlarged the synergistic effect and/or interfacial effect between MnO2nanosheets and Au-NPs and facilitated the uptake of electrons by MnO2from MB during the oxidation,thus validating the application of MnO2/Au-NPs nanocomposite for direct removal of organic dyes from wastewater in a simple and convenient fashion.

关键词： MnO2/Au-NPs nanocomposite In-situ generation Dye degradation Synergistic effect and inteffacial effect Enhanced oxidative degradation

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全球清洁能源快速增长引发对土地资源占用的担忧

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science Bulletin 2023年第6期68卷 571-573,M0003页

作者：张宁段华波杨家宽 Leibniz Institute of ecological Urban and Regional Development(IOER) Dresden 01217Germany school of environmental science&Engineering Huazhong University of Science and Technology(HUST)Wuhan 430074China

Most countries in the world have joined the race for carbon neutrality, to meet the goals of the 2015 Paris Agreement, leading to a boom in the clean-energy sector. However, the construction of clean-energy infrastructure can disproportionately occupy limited productive soil and natural land resources, compared to conventional energy plants (Fig. 1). Thus, comprehending the land footprint resulting from the proliferation of clean-energy systems is now imperative, to better anticipate and manage the energy industry, and specifically to quantify the land-use trade-offs of the energy transition in a global context.

关键词： occupy neutral goals

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Ti-Fe_(2)O_(3)/Ni(OH)_(x) as an efficient and durable photoanode for the photoelectrochemical catalysis of PET plastic to formic acid

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Journal of Energy Chemistry 2023年第3期78卷 487-496,I0014页

作者： Xin Li Jianying Wang Mingze Sun Xufang Qian Yixin Zhao school of environmental science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China Shanghai Institute of Pollution Control and ecological Security Shanghai 200240China

Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity,selectivity and long-term durability are required for the future up-scaling industrial applications.Herein,we employed the interfacial modification strategy to develop an efficient and stable photoanode and evaluated its PEC activity for ethylene glycol(EG,derived from PET hydrolysate) oxidation to formic acid.The interfacial modification between Fe_(2)O_(3)semiconductor and Ni(OH)xcocatalyst with ultrathin TiO_(x) interlayer not only improved the photocurrent density by accelerating the kinetics of photogenerated charge carriers,but also kept the high Faradaic efficiency(over 95% in 30 h) towards the value-added formic acid product.This work proposes an effective method to promote the PEC activity and enhance the long-term stability of photoelectrodes for upcycling PET plastic wastes.

关键词： Plastic waste Formic acid Photoelectrochemical catalysis High durability Interfacial modiﬁcation

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Hierarchical Ag-SiO_2@Fe_3O_4magnetic composites for elemental mercury removal from non-ferrous metal smelting flue gas

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Journal of environmental sciences 2019年第5期31卷 111-120页

作者： Yongpeng Ma Bailong Mu Xiaojing Zhang Hongzhong Zhang Haomiao Xu Zan Qu Li Gao Henan Collaborative Innovation Center of environmental Pollution Control and ecological Restoration School of Material and Chemical Engineering Zhengzhou University of Light Industry school of environmental science and Engineering Shanghai Jiao Tong University College of Resources and environmental science Ningxia University

Hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites were selected for elemental mercury(Hg^0) removal from non-ferrous metal smelting flue gas in this study. Results showed that the hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites had favorable Hg^0 removal ability at low temperature. Moreover, the adsorption capacity of hierarchical magnetic composite is much larger than that of pure Fe_3O_4 and SiO_2@Fe_3O_4. The Hg^0 removal efficiency reached the highest value as approximately 92% under the reaction temperature of 150°C, while the removal efficiency sharply reduced in the absence of O_2. The characterization results indicated that Ag nanoparticles grew on the surface of SiO_2@Fe_3O_4 support. The large surface area of SiO_2 supplied efficient reaction room for Hg and Ag atoms. Ag–Hg amalgam is generated on the surface of the composites. In addition, this magnetic material could be easily separated from fly ashes when adopted for treating real flue gas, and the spent materials could be regenerated using a simple thermal-desorption method.

关键词： Elemental mercury Silver nanoparticles Magnetic composites Non-ferrous metal Flue gas

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Partial aging can counter-intuitively couple with sulfidation to improve the reactive durability of zerovalent iron

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Frontiers of environmental science & Engineering 2024年第2期18卷 1-11页

作者： Yiwei Liu Kaili Gu Jinhua Zhang Jinxiang Li Jieshu Qian Jinyou Shen Xiaohong Guan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China School of Ecological and Environmental Sciences East China Normal UniversityShanghai 200241China

Sulfated zero-valent iron(SZVI)has shown promising applications in wastewater treatment.However,the rapid decline in the reactivity of SZVI with time limits its real practice.To mediate this problem,partial aging was proposed to improve the reactive durability of SZVI.Taking Cr(VI)as the target contaminant,we found that the aged ZVI(AZVI)gradually lost reactivity as aging time increased from 0.5 to 2 d.Counter-intuitively,the partially aged SZVI(ASZVI)showed greater reactivity than SZVI when exposed to oxygenated water for a period ranging from 0.5 to 14 d.In addition,the ASZVI with 0.5 d of aging time(ASZVI-0.5)not only maintained reactivity in successive runs but also increased the Cr(VI)removal capacity from 9.1 mg/g by SZVI to 19.1 mg/g by ASZVI-0.5.Correlation analysis further revealed that the electron transfer from the Fe0 core to the shell was mediated by the conductive FeS and FeS2 in the subshell of ASZVI.Meanwhile,the lepidocrocite and magnetite on the surface of ASZVI facilitated Cr(VI)adsorption and subsequent electron transfer for Cr(VI)reduction.Moreover,the iron(hydr)oxide shell could retain the conductive FeS and FeS2 in the subshell,allowing ASZVI to reduce Cr(VI)efficiently and sustainably.In general,partial aging can enhance the reactive durability of ZVI when coupled with sulfidation and this synergistic effect will be beneficial to the application of SZVI-based technology for wastewater treatment.

关键词： Zerovalent iron Sulfidation Partial aging Interface reconstruction Electron transfer

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