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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 results.In 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/L.Meanwhile,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 time.In addition,alkaline conditions(pH≥8.0)inhibited CFA and BZF degradations,while nonacidic pH(pH≥7.0)remarkably inhibited SMX degradation.Results of the kinetic model indicated the formation of phosphate(H_(2)PO_(4)^(·)/HPO_(4)^(·-))and/or carbonate radicals(CO_(3)^(·-))could limit pharmaceutical removal.The 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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Ferrihydrite transformation impacted by coprecipitation of lignin:Inhibition or facilitation?

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Journal of Environmental Sciences 2024年第5期139卷 23-33页

作者： Lin Liu Zhihui Yang Weichun Yang Wen Jiang Qi Liao Mengying Si Feiping Zhao School of metallurgy and Environment Central South UniversityChangsha 410083China Chinese national engineering research center for control&treatment of heavy metal pollution(CNERC-CTHMP) Changsha 410083China

Lignin is a common soil organic matter that is present in soils,but its effect on the transformation of ferrihydrite(Fh)remains unclear.Organic matter is generally assumed to inhibit Fh transformation.However,lignin can reduce Fh to Fe(Ⅱ),in which Fe(Ⅱ)-catalyzed Fh transformation occurs.Herein,the effects of lignin on Fh transformation were investigated at 75℃ as a function of the lignin/Fh mass ratio(0-0.2),pH(4-8)and aging time(0-96 hr).The results of Fh-lignin samples(mass ratios=0.1)aged at different pH values showed that for Fh-lignin the time of Fh transformation into secondary crystalline minerals was significantly shortened at pH 6 when compared with pure Fh,and the Fe(Ⅱ)-accelerated transformation of Fh was strongly dependent on pH.Under pH 6,at low lignin/Fh mass ratios(0.05-0.1),the time of secondary mineral formation decreased with increasing lignin content.For high lignosulfonate-content material(lignin:Fh=0.2),Fh did not transform into secondary minerals,indicating that lignin content plays a major role in Fh transformation.In addition,lignin affected the pathway of Fh transformation by inhibiting goethite formation and facilitating hematite formation.The effect of coprecipitation of lignin on Fh transformation should be useful in understanding the complex iron and carbon cycles in a soil environment.

关键词： Ferrihydrite transformation Lignin Hematite Goethite Fe(Ⅱ)-catalyzed Reactive Fe(Ⅲ)species

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Migration and distribution characteristics of soil heavy metal(loid)s at a lead smelting site

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Journal of Environmental Sciences 2024年第1期135卷 600-609页

作者： Chuxuan Li Mu Li Jiaqing Zeng Shanxin Yuan Xinghua Luo Chuan Wu Shengguo Xue School of metallurgy and Environment Central South UniversityChangsha 410083China Chinese national engineering research center for control and treatment of heavy metal pollution Central South UniversityChangsha 410083China

heavy metal(loid)s contamination is a constant issue at smelting sites.It is essential to investigate the spatial distribution and migration characteristics of heavy metal(loid)s in the soil for environmental management and remediation strategies of non-ferrous smelting sites.In this study,203 soil samples from 57 sites were collected in a typical lead smelting site.The findings demonstrated that there were significant Pb,Zn,Cd,and As contamination in soil samples.The spatial distribution of heavy metal(loid)s showed strong spatial heterogeneity,the contaminated soil areas of Pb,As,Cd,and Zn were 99.5%,98.9%,85.3%,and 72.4%,respectively.Pb,Cd,and As contamination of the soil reached a depth of 5 m,which migrated from the surface to deep soil layers.The leaching contents of Zn,Pb,and As decreased obviously in 3-4 m soil layer,but the leaching content of Cd was still high,which indicated the high migration of Cd.With the increase of depth,the proportion of acid soluble fraction of heavy metal(loid)s decreased,and the residual fraction increased.The acid soluble fraction of Cd accounted for a higher proportion,and As mainly existed in reducible and residual fractions in soil.According to the calculation of the migration factor,the migration of heavy metal(loid)s in soils were ordered as Cd>Zn>Pb>As.The outcomes are advantageous for risk reduction and site remediation for non-ferrous metal smelting sites.

关键词： Smelting sites heavy metal(loid)s Spatial distribution Chemical speciation Migration characteristics

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Progress of gaseous arsenic removal from flue gas by adsorption:Experimental and theoretical calculations

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Journal of Environmental Sciences 2024年第2期136卷 470-485页

作者： Xuelei Yan Qingzhu Li Xiaowei Huang Bensheng Li Shengtu Li Qingwei Wang School of metallurgy and Environment Central South UniversityChangsha 410083China national engineering research Centre for control and treatment of heavy metal pollution Central South UniversityChangsha 410083China national engineering research center for Rare Earth Materials General Research Institute for Non-Ferrous MetalsBeijing 100088China

Because of its high mobility and difficult capture,gaseous arsenic pollution control has become the focus of arsenic pollution control.It mainly exists in the form of highly toxic As_(2)O_(3)in the flue gas.Therefore,removing gaseous As_(2)O_(3)from flue gas is of great practical significance for arsenic pollution control.Stabilizing gaseous As_(2)O_(3)on the surface of adsorbents by physical or chemical adsorption is an effective way to reduce the content of arsenic in the flue gas and alleviate arsenic pollution.Over the past few decades,various adsorbents have been developed to capture gaseous As_(2)O_(3)in the flue gas,and their adsorption mechanisms have been studied in detail.Thus,it is necessary to review the strategies of arsenic removal from flue gas by adsorption,which can inspire further research.Based on summarizing the morphological distribution of gaseous As_(2)O_(3)in the flue gas,this review further summarizes the removal of gaseous As_(2)O_(3)by several adsorbents and the effect of temperature and the main components of the flue gas on arsenic adsorption.In addition,the mechanism of arsenic removal based on adsorption in the flue gas is discussed in depth through theoretical calculations,which is the particular focus of this review.Finally,prospects based on the present research state of arsenic removal by adsorption are proposed to provide ideas for developing effective and stable adsorbents for arsenic removal from flue gas.

关键词： Gaseous arsenic Flue gas Adsorption Theoretical calculation Mechanism

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A review on the transformation of birnessite in the environment:Implication for the stabilization of heavy metals

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Journal of Environmental Sciences 2024年第5期139卷 496-515页

作者： Miao Shi Qingzhu Li Qingwei Wang Xuelei Yan Bensheng Li Linhai Feng Chao Wu Rongrong Qiu Hongkai Zhang Zhihui Yang Weichun Yang Qi Liao Liyuan Chai School of metallurgy and Environment Central South UniversityChangsha 410083China national engineering research Centre for control and treatment ofheavy metal pollution Central South UniversityChangsha 410083China Water pollution control technology Key Lab of Hunan Province Changsha 410083China

Birnessite is ubiquitous in the natural environment where heavy metals are retained and easily transformed.The surface properties and structure of birnessite change with the changes in external environmental conditions,which also affects the fate of heavy metals.Clarifying the effect and mechanism of the birnessite phase transition process on heavy metals is the key to taking effective measures to prevent and control heavy metal pollution.Therefore,the four transformation pathways of birnessite are summarized first in this review.Second,the relationship between transformation pathways and environmental conditions is proposed.These relevant environmental conditions include abiotic(e.g.,co-existing ions,pH,oxygen pressure,temperature,electric field,light,aging,pressure)and biotic factors(e.g.,microorganisms,biomolecules).The phase transformation is achieved by the key intermediate of Mn(Ⅲ)through interlayer-condensation,folding,neutralizationdisproportionation,and dissolution-recrystallization mechanisms.The AOS(average oxidation state)of Mn and interlayer spacing are closely correlated with the phase transformation of birnessite.Last but not least,the mechanisms of heavy metals immobilization in the transformation process of birnessite are summed up.They involve isomorphous substitution,redox,complexation,hydration/dehydration,etc.The transformation of birnessite and its implication on heavy metals will be helpful for understanding and predicting the behavior of heavy metals and the crucial phase of manganese oxides/hydroxides in natural and engineered environments.

关键词： Birnessite Transformation heavy metals Pathways Mechanism

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Feasibility of low-intensity ultrasound treatment with hydroxylamine to accelerate the initiation of partial nitrification and allow operation under intermittent aeration

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Journal of Environmental Sciences 2024年第5期139卷 446-459页

作者： Jianxiong Jian Xiaojian Liao Zhihua Mo Shoupeng Li Lei Li Shaojin Chen Zhenhua Huang Junhao Chen Wencan Dai Shuiyu Sun Guangzhou Key Laboratory Environmental Catalysis and pollution control Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangdong Province Solid Waste Recycling and heavy metal pollution control engineering technology research center Guangdong Polytechnic of Environmental Protection EngineeringFoshan 528216China Analysis and Test center Guangdong University of TechnologyGuangzhou 510006China

Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant group.Collectively,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.

关键词： Partial nitrification Low-intensity ultrasound Hydroxylamine Ammonia oxidizing bacteria Nitrite oxidizing bacteria

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Nanosize-effect on the distribution of heavy metals in copper smelting dust:Based on sophisticated dust sorting approach

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Nano research 2024年第1期17卷 312-320页

作者： Ken Li Zuwu Liao Hengdi Ye Qingzhu Li Fenghua Shen Qian Li Hui Liu Qingwei Wang Xu Yan Zhang Lin Liyuan Chai School of metallurgy and Environment Central South UniversityChangsha 410083China Chinese national engineering research center for control&treatment of heavy metal pollution Changsha 410083China national engineering research center of Sintering and Pelletizing Equipment System Zhongye Changtian International Engineering Co.LtdChangsha 410205China

Dust particles emitted from smelters can be hazardous to ecosystems and humans,as they are often enriched in metallic compounds.Here,we combined multi-method mineralogical analysis with a sophisticated size sorting approach for copper smelting dust to study the nanosize-effect on heavy metal distribution,which has hitherto been underestimated.Three types of dust were collected from a copper flash smelter and then size-sorted using a Dekati low-pressure impactor.Results showed that all three samples could easily sort out nanoscale dust particles(heavy metals(Pb,Zn,Cu,and As)and their mineral species in dust was examined at various particle sizes.It was discovered that different heavy metals are enriched on nanoparticles in specific sizes.In micron-sized particles,heavy metals are generally found in discrete phases(e.g.,CuSO_(4),PbSO_(4),and As_(2)O_(3)).In nanoscale particles,the dominant phase is Fe_(3)O_(4),while heavy metals are mostly found in lattice substitution(e.g.,CuFe_(2)O_(4)and ZnFe_(2)O_(4)).Two distinct nano-dust morphologies were found:One with irregular mesh or chain structures consisting of particles of a few nanometers,and the other with polygonal crystals in larger sizes of hundreds of nanometers.The enrichment of heavy metals in the latter morphology is more pronounced,possibly because lattice substitution of heavy metals is more likely to occur when polycrystalline particles are formed.

关键词： copper flue dust size-sorted heavy metal distribution morphology nano-sized effects

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Geochemical fractionation and potential release behaviour of heavy metals in lead–zinc smelting soils

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Journal of Environmental Sciences 2024年第5期139卷 1-11页

作者： Xinghua Luo Chao Xiang Chuan Wu Wenyan Gao Wenshun Ke Jiaqing Zeng Waichin Li Shengguo Xue School of metallurgy and Environment Central South UniversityChangsha 410083China Chinese national engineering research center for control and treatment of heavy metal pollution Central South UniversityChangsha 410083China Department of Science and Environmental Studies The Education University of Hong KongHong Kong 999077China

The lack of understanding of heavy metal speciation and solubility control mechanisms in smelting soils limits the effective pollution control.In this study smelting soils were investigated by an advanced mineralogical analysis(AMICS),leaching tests and thermodynamic modelling.The aims were to identify the partitioning and release behaviour of Pb,Zn,Cd and As.The integration of multiple techniques was necessary and displayed coherent results.In addition to the residual fraction,Pb and Zn were predominantly associated with reducible fractions,and As primarily existed as the crystalline iron oxide-bound fractions.AMICS quantitative analysis further confirmed that Fe oxyhydroxides were the common dominant phase for As,Cd,Pb and Zn.In addition,a metal arsenate(paulmooreite)was an important mineral host for Pb and As.The pH-stat leaching indicted that the release of Pb,Zn and Cd increased towards low pH values while release of As increased towards high p H values.The separate leaching schemes were associated with the geochemical behaviour under the control of minerals and were confirmed by thermodynamic modelling.PHREEQC calculations suggested that the formation of arsenate minerals(schultenite,mimetite and koritnigite)and the binding to Fe oxyhydroxides synchronously controlled the release of Pb,Zn,Cd and As.Our results emphasized the governing role of Fe oxyhydroxides and secondary insoluble minerals in natural attenuation of heavy metals,which provides a novelty strategy for the stabilization of multi-metals in smelting sites.

关键词： Smelting soils heavy metal Fractionation AMICS Geochemical modelling

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Efficient removal of natural organo-chromium(Ⅲ)through selfcirculating decomplex and immobilization with nanoscale zerovalent iron

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Nano research 2024年第1期17卷 364-371页

作者： Zhicheng Dong Yunyun Xu Can Wu Jin Chao Chen Tian Zhang Lin School of metallurgy and Environment Central South UniversityChangsha 410083China Chinese national engineering research center for control&treatment of heavy metal pollution Changsha 410083China College of Ecology and Environment Chengdu University of TechnologyChengdu 610059China School of Environment and Energy The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters(Ministry of Education)South China University of TechnologyGuangzhou 510006China

Organo-chromium(III)complex is one of the chromium contaminant species,which would transform to high-toxic Cr(VI)during migrating in the environment.Such natural organo-chromium(III)(NOCr)is difficult to remove by traditional degradation or precipitation methods,due to its high stability and solubility.Herein,we demonstrated a novel NOCr removing method by transforming it to certain structures similar to Cr-Fe minerals in nature,through a self-circulating decomplex and immobilization mechanism with nano zero-valent iron(nZVI).Taking chromium glycinate(Cr-Gly)as a probe,nZVI showed a high Cr removal efficiency of 99.4%under ambient conditions.The removal process included three stages of adsorption,decomplexation,and re-immobilization.Cr-Gly was first adsorbed on the surface of nZVI by chemisorption of the oxide shell.Then,the adsorbed Cr-Gly was decomplexed and oxidized to Cr(VI)by·OH and 1O_(2),which were generated from molecular oxygen activated by nZVI.Meanwhile,the released Cr(VI)could be in-situ adsorbed and re-reduced to Cr(III),which was further immobilized in form of Cr-O-Fe complex.As the Cr-O-Fe complexing structure was similar to that of Cr-Fe minerals(such as chromohercynite)in nature,this work explored a novel and efficient NOCr removing method that was potential to weaken chromium pollution in the environment.

关键词： organo-chromium(III) zero-valent iron adsorption decomplexation Cr immobilization

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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 challenge.In 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-FeOOH.Functioning as a hole extraction layer,needle-leaf-likeβ-FeOOH can facilitate efficient hole migration and enhance charge transport.Remarkably,the optimized 0.2-pg-C_(3)N_(4)/β-FeOOH could degrade 78%of ofloxacin(OFLO)in 90 min.The 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 cathode.Consequently,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 pollutants.Experimental and theoretical calculation results underscore that this investigation is grounded in a distinctive electron and hole dual channel transfer mechanism.These 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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