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Factors hindering the degradation of pharmaceuticals from human urine in an iron-activated persulfate system

Journal of Environmental Sciences 2024年第1期135卷 130-148页

作者： Yiruiwen Xie Dao Guan Yangfan Deng Yugo Sato Yu Luo Guanghao Chen Department of Civil and Environmental engineering Water Technology LabHong Kong Branch of Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science&TechnologyHong Kong 999077China

This study investigated the degradation of clofibric acid(CFA),bezafibrate(BZF),and sulfamethoxazole(SMX)in synthetic human urine using a novel mesoporous iron powderactivated persulfate system(mFe-PS system),and identified the factors limiting their degradation in synthetic human urine.A kinetic model was established to expose the radical production in various reaction conditions,and experiments were conducted to verify the modeling *** the phosphate-containing mFe-PS system,the 120 min removal efficiency of CFA decreased from 95.1%to 76.6%as the phosphate concentration increased from 0.32 to 6.45 mmol/L,but recovered to 90.5%when phosphate concentration increased to 16.10 mmol/***,the increased concentration of phosphate from 0.32 to 16.10mmol/L reduced the BZF degradation efficacy from 91.5%to 79.0%,whereas SMX removal improved from 37.3%to 62.9%.The m Fe-PS system containing(bi)carbonate,from 4.20 to166.70 mmol/L,reduced CFA and BZF removal efficiencies from 100%to 76.8%and 80.4%,respectively,and SMX from 83.5%to 56.7%within a 120-min reaction *** addition,alkaline conditions(pH≥8.0)inhibited CFA and BZF degradations,while nonacidic pH(pH≥7.0)remarkably inhibited SMX *** of the kinetic model indicated the formation of phosphate(H_(2)PO_(4)^(·)/HPO_(4)^(·-))and/or carbonate radicals(CO_(3)^(·-))could limit pharmaceutical *** transformation products(TPs)of the pharmaceuticals revealed more incompletely oxidized TPs occurred in the phosphate-and(bi)carbonate-containing m Fe-PS systems,and indicated that H_(2)PO_(4)^(·)/HPO_(4)^(·-)mainly degraded pharmaceuticals via a benzene ring-opening reaction while CO_(3)^(·-)preferentially oxidized pharmaceuticals via a hydroxylation reaction.

关键词： Pharmaceutical degradation Human urine Iron-activated persulfate system Phosphate radicals Carbonate radicals Transformation products

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Photoelectrocatalytic hydrogen evolution and synchronous degradation of organic pollutants by pg-C_(3)N_(4)/β-FeOOH S-scheme heterojunction

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Science China(Technological Sciences) 2024年第4期67卷 1238-1252页

作者： LI XiBao HAN Tao ZHOU YingTang XIE Yu LUO YiDan HUANG JunTong CHEN Zhi DENG Fang School of Materials Science and engineering Nanchang Hangkong UniversityNanchang 330063China National-Local Joint engineering Research center of heavy metal Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316022China

Crafting photoelectrocatalytic materials with robust oxidation-reduction properties for simultaneous hydrogen evolution and pollutant degradation poses a formidable *** this study,a pg-C_(3)N_(4)/β-FeOOH S-scheme heterostructure with a special energy band structure was developed by anchoring porous pg-C_(3)N_(4)on needle shapedβ-*** as a hole extraction layer,needle-leaf-likeβ-FeOOH can facilitate efficient hole migration and enhance charge ***,the optimized 0.2-pg-C_(3)N_(4)/β-FeOOH could degrade 78%of ofloxacin(OFLO)in 90 *** organic pollutants could absorb a large number of holes,which prompted a greater proportion of photogenerated electrons to actively participate in the hydrogen evolution reaction at the ***,the hydrogen production of 0.2-pg-C_(3)N_(4)/β-FeOOH reached 1452.88μmol cm^(-2)h^(-1),exhibiting a notable increase of 61.81-165.12μmol cm^(-2)h^(-1)compared with that in the absence of *** and theoretical calculation results underscore that this investigation is grounded in a distinctive electron and hole dual channel transfer *** findings offer novel insights for the future development of S-scheme heterojunction photoelectrocatalytic materials capable of concurrently degrading pollutants and promoting hydrogen evolution.

关键词： photoelectrocatalysis hydrogen evolution degradation synchronous S-scheme heterojunction

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Selective recovery of Th(Ⅳ) from radioactive rare earth waste residue by utilizing MoS_(2)-modified ion-absorbed type rare earth tailings

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Journal of Rare Earths 2024年第9期42卷 1782-1791,I0005页

作者： Xirong Chen Xinyu Fu Yun Gao Zhiyuan Zeng Bin Huang Xiaoqi Sun Faculty of Materials metallurgy and Chemistry Jiangxi University of Science and TechnologyGanzhou341000China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Fujian Research center for Rare Earth engineering technology Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen361021China Fujian College University of Chinese Academy of SciencesFuzhou350002China Jiangxi Province Key Laboratory of cleaner production of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhouJiangxi341000China

In the process of extracting ion-absorbed rare earth ore(IREO),the production of radioactive waste is a major environmental *** address this issue,MoS_(2) was used to modify ion-absorbed rare earth tailings(RET) to synthesize a novel MoS_(2)@RET composite material for the effective handling of radioactive waste generated in IREO separation *** composite material was thoroughly characterized using various analytical techniques,including X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),thermogravimetry(TG),Fourier-transform infrared(FTIR),scanning electron microscopy(SEM),Brunaue r-Emmett-Teller(BET) and energy dispersive spectroscopy(EDS).By optimizing the operating parameters,the optimal experimental conditions were determined to be pH=3,contact time=60 min,liquid-solid ratio=6 g/L,and initial concentration=150 mg/*** adsorption data fitted well with the pseudo second-order rate *** thermodynamic parameters concerning the adsorption of Th(Ⅳ) were analyzed and *** isotherm model is a more fitting choice for the adsorption process compared to the Freundlich isotherm ***_(2)@RET was used in the acid leachate of IREO waste residue,achieving the separation of Th and rare earth *** mechanism of Th(Ⅳ) adsorption by MoS_(2)@RET was investigated,revealing that the adsorption process involves electrostatic interactions,chemical bonding,and redox *** above research results indicate that MoS_(2)@RET composite materials have application potential in the sustainable treatment of IREO radioactive waste.

关键词： Rare earths Thorium Radioactive waste residue Adsorption Separation

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A Non-Contact Original-State Online Real-Time Monitoring Method for Complex Liquids in Industrial Processes

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engineering 2018年第3期4卷 392-397页

作者： Ning Duan Linhua Jiang Fuyuan Xu Ge Zhang center for heavy metal cleaner production engineering technology Chinese Research Academy of Environmental Sciences Beijing 100012 China

Failures are very common during the online real-time monitoring of large quantities of complex liquids in industrial processes, and can result in excessive resource consumption and pollution. In this study, we introduce a monitoring method capable of non-contact original-state online real-time monitoring for strongly coated, high-salinity, and multi-component liquids. The principle of the method is to establish the relationship among the concentration of the target substance in the liquid （C）, the color space coor- dinates of the target substance at different concentrations （L＊, a＊, b＊）, and the maximum absorption wave- length （λmax）; subsequently, the optimum wavelength λT of the liquid is determined by a high-precision scanning-type monitoring system that is used to detect the instantaneous concentration of the target substance in the flowing liquid. Unlike traditional monitoring methods and existing online monitoring methods, the proposed method does not require any pretreatment of the samples （i.e., filtration, dilution, oxidation/reduction, addition of chromogenic agent, constant volume, etc.）, and it is capable of original- state online real-time monitoring. This method is employed at a large electrolytic manganese plant to monitor the Fe3. concentration in the colloidal process of the plant＇s aging liquid （where the concentra- tions of Fe3＋, Mn2＋, and （NH4）2SO4 are 0.5-18 mg.L 1, 35-39 g.L 1, and 90-110 g.L 1, respectively）. The relative error of this monitoring method compared with an off-line laboratory monitoring is less than 2%.

关键词： Complex liquid Original-state monitoring Online real-time Non-contact identification

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Direct Regeneration of Spent Lithium-Ion Battery Cathodes:From Theoretical Study to production Practice

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Nano-Micro Letters 2024年第10期16卷 304-336页

作者： Meiting Huang Mei Wang Liming Yang Zhihao Wang Haoxuan Yu Kechun Chen Fei Han Liang Chen Chenxi Xu Lihua Wang Penghui Shao Xubiao Luo National-Local Joint engineering Research center of heavy metals Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063People's Republic of China Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials School of Chemistry and Chemical EngineeringHunan Institute of Science and TechnologyYueyang 414006People's Republic of China College of Materials Science and engineering Central South University of Forestry and TechnologyChangsha 410004People's Republic of China School of Life Science Jinggangshan UniversityJi'an 343009People's Republic of China

Direct regeneration method has been widely concerned by researchers in the field of battery recycling because of its advantages of in situ regeneration,short process and less pollutant *** this review,we firstly analyze the primary causes for the failure of three representative battery cathodes(lithium iron phosphate,layered lithium transition metal oxide and lithium cobalt oxide),targeting at illustrating their underlying regeneration mecha-nism and *** stripping of material from the collector to obtain pure cathode material has become a first challenge in recycling,for which we report several pretreatment methods currently available for subsequent regeneration *** review and discuss emphatically the research progress of five direct regeneration methods,including solid-state sintering,hydrothermal,eutectic molten salt,electrochemical and chemical lithiation ***,the application of direct regeneration technology in production practice is introduced,the problems exposed at the early stage of the industrialization of direct regeneration technol-ogy are revealed,and the prospect of future large-scale commercial production is *** is hoped that this review will give readers a comprehensive and basic understanding of direct regeneration methods for used lithium-ion batteries and promote the industrial application of direct regeneration technology.

关键词： Spent LIBs Failure reasons Cathode recycling Direct regeneration production practice

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Recent process developments in beneficiation and metallurgy of rare earths:A review

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Journal of Rare Earths 2024年第4期42卷 629-642页

作者： Shaokai Cheng Wenbo Li Yuexin Han Yongsheng Sun Peng Gao Xiaolong Zhang School of Resources and Civil engineering Northeastern UniversityShenyang110819China National-local Joint engineering Research center of High-efficient Exploitation technology for Refractory Iron Ore Resources Shenyang110819China

Rare earth elements(REEs)are irreplaceable materials supporting low-carbon technology and equip-ment,and their commercial demand and strategic position are becoming increasingly *** the continuous depletion of rare earth(RE)resources,developing high-efficiency beneficiation and eco-friendly metallurgical processes has attracted widespread *** paper reviews the major minerals exploited for RE production and their deposits,as well as the beneficiation and metallurgical processes of RE ***,monazite,mixed RE ores,and ion-adsorption clays are the main raw materials in the world to ***-bearing ores(except ion-adsorption minerals)are generally beneficiated by flotation,gravity and magnetic separation *** mainstream metallurgical processes for bastnaesite,monazite and mixed RE concentrates are oxidation roasting-HCl leaching,caustic soda decomposition and high-temperature concentrated sulfuric acid roasting,***-adsorption clays are directly processed by in situ leaching-precipitation/solvent *** achieve the sustainable development of RE resources,it is essential to further explore innovative techniques to achievecomprehensive utilization and cleaner production.

关键词： Rare earths Beneficiation processes metallurgical processes cleaner production

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Reductive recovery of manganese from low-grade manganese dioxide ore using toxic nitrocellulose acid wastewater as reductant

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International Journal of Minerals,metallurgy and Materials 2018年第9期25卷 990-999页

作者： Yong-tao Zhang Zhi-gang Dan Ning Duan Bao-ping Xin School of Petroleum and Environment engineering Yan'an University School of Materials Science & engineering Beijing Institute of Technology technology center for heavy metal cleaner production engineering Chinese Research Academy of Environmental Sciences

The hydrometallurgical strategy of extracting Mn from low-grade Mn ores has attracted attention for the production of electrolytic manganese metal(EMM). In this work, the reductive dissolution of low-grade Mn O2 ores using toxic nitrocellulose acidic wastewater(NAW) as a reductant was investigated for the first time. Under the optimized conditions of an Mn O2 ore dosage of 100 g·L-1, an ore particle size of-200 mesh, concentrated H2 SO4-to-NAW volume ratio of 0.12, reaction temperature of 90°C, stirring speed at 160 r·min-1, and a contact time of 120 min, the reductive leaching efficiency of Mn and the total organic carbon(TOC) removal efficiency of NAW reached 97.4% and 98.5%, respectively. The residual TOC of 31.6 mg·L-1 did not adversely affect the preparation of EMM. The current process offers a feasible route for the concurrent realization of the reductive leaching of Mn and the treatment of toxic wastewater via a simple one-step process.

关键词： low-grade manganese dioxide ore nitrocellulose acid wastewater sulfuric acid leaching Mn reductive dissolution electrolytic manganese metal

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A cascade of in situ conversion of bicarbonate to CO_(2) and CO_(2) electroreduction in a flow cell with a Ni-N-S catalyst

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Journal of Energy Chemistry 2024年第1期88卷 183-193,I0005页

作者： Linghui Kong Min Wang Yongxiao Tuo Shanshan Zhou Jinxiu Wang Guangbo Liu Xuejing Cui Jiali Wang Luhua Jiang Nanomaterials and Electrocatalysis Laboratory College of Materials Science and EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina State Key Laboratory of heavy Oil Processing College of New EnergyChina University of Petroleum(East China)Qingdao 266580ShandongChina

Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high *** electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode ***,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow *** a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is *** experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)*** a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni *** importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid *** work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.

关键词： S doped Ni-N-C single atom catalysts CO_(2)electrochemical reduction DFT calculations Membrane electrode assembly Reduction of bicarbonate

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Effect of tillage state of paddy soils with heavy metal pollution on the nosZ gene of N_(2)O reductase

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Journal of Environmental Sciences 2024年第3期137卷 469-477页

作者： Liping Jiang Shiguang Liu Shanyun Wang Libo Sun Guibing Zhu Key Laboratory of Drinking Water Science and technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China School of Environmental and Civil engineering Jiangnan UniversityWuxi 214122China

Paddy soils are an important source of atmospheric nitrous oxide(N_(2)O).However,numerous studies have focused on N_(2)O production during the soil tillage period,neglecting the N_(2)O production during the dry fallow *** this study,we conducted an incubation experiment using the acetylene inhibition technique to investigate N_(2)O emission and reduction rates of paddy soil profiles(0-1 m)from Guangdong Province and Jinlin Province in China,with different heavy-metal pollution *** abundance and community structures of denitrifying bacteria were determined via quantitative-PCR and Illumina MiSeq sequencing of nosZ,nirK,and nirS *** results showed that the potential N_(2)O emission rate,N_(2)O production rate,and denitrification rate have decreased with increasing soil vertical depth and heavy-metal *** importantly,we found that the functional gene type of N_(2)O reductase switched with the tillage state of paddy soils,which cladeⅡnos Z genes were the dominant gene during the tillage period,while cladeⅠnos Z genes were the dominant gene during the dry fallow *** heavy-metal pollution has less effect on the niche differentiation of the nos Z *** N_(2)O emission rate was significantly regulated by the genus Bradyhizobium,which contains both N_(2)O reductase and nitrite reductase *** findings suggests that the nos Z gene of N_(2)O reductase can significantly impact the N_(2)O emission from paddy soils.

关键词： Pappy soils N_(2)O reductase nosZ gene heavy-metal pollution

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Adsorption and desorption of SO_2, NO and chlorobenzene on activated carbon

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Journal of Environmental Sciences 2016年第5期28卷 128-135页

作者： Yuran Li Yangyang Guo Tingyu Zhu Song Ding Beijing engineering Research center of Process Pollution Control National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Institute of Process Engineering Chinese Academy of Sciences

Activated carbon（AC） is very effective for multi-pollutant removal; however, the complicated components in flue gas can influence each other＇s adsorption. A series of adsorption experiments for multicomponents, including SO_2, NO, chlorobenzene and H2 O,on AC were performed in a fixed-bed reactor. For single-component adsorption, the adsorption amount for chlorobenzene was larger than for SO_2 and NO on the AC. In the multi-component atmosphere, the adsorption amount decreased by 27.6% for chlorobenzene and decreased by 95.6% for NO, whereas it increased by a factor of two for SO_2,demonstrating that a complex atmosphere is unfavorable for chlorobenzene adsorption and inhibits NO adsorption. In contrast, it is very beneficial for SO_2 adsorption. The temperature-programmed desorption（TPD） results indicated that the binding strength between the gas adsorbates and the AC follows the order of SO_2〉 chlorobenzene 〉 NO. The adsorption amount is independent of the binding strength. The presence of H2 O enhanced the component effects, while it weakened the binding force between the gas adsorbates and the AC. AC oxygen functional groups were analyzed using TPD and X-ray photoelectron spectroscopy（XPS） measurements. The results reveal the reason why the chlorobenzene adsorption is less affected by the presence of other components. Lactone groups partly transform into carbonyl and quinone groups after chlorobenzene desorption. The chlorobenzene adsorption increases the number of C = O groups, which explains the positive effect of chlorobenzene on SO_2 adsorption and the strong NO adsorption.

关键词： Activated carbon Multi-components Functional groups Binding force Flue gas

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