Microplastics(MPs)are ubiquitous and pose an environmental risk.This review examined MP pollution in terrestrial ecosystems from a myriad of poorly understood sources.Knowledge regarding the occurrence sources,migrati...Microplastics(MPs)are ubiquitous and pose an environmental risk.This review examined MP pollution in terrestrial ecosystems from a myriad of poorly understood sources.Knowledge regarding the occurrence sources,migration behaviors,ecotoxicology,absorption mechanisms,and effects of MPs has also been fully summarized.Microplastics interact with contaminants,such as antibiotics,pesticides,heavy metals,etc.,and may act as vectors for contaminant transfer in terrestrial ecosystems.The transportation and retention of MPs in soil are governed by interactions among their inherent properties,such as size,shape,surface charge,and density.Interestingly,MP migration into soil is lacking research.The MPs and nanoplastics were also found in edible fruits and vegetables.The MP contamination in soil affects ecosystems,causing soil structure changes,fertility reduction,and pollutant leaching into groundwater.The MP concentration lies in the range of 43-2443 and 40-43000 items kg-1in agricultural and urban soils,respectively.This review provides a comprehensive roadmap for future research and a framework for soil MP risk assessment.Future studies on the uptake,accumulation,and translocation of MPs and their associated toxins by plants are essential for evaluating their risks to food security and human health.Research on MPs in terrestrial habitats lacks comprehensive data on their long-term persistence,degradation pathways,and interactions with soil components under varying environmental conditions.Additionally,limited understanding exists regarding MP impacts on soil biodiversity,pollutant mobility,and plant uptake,highlighting the need for innovative detection methods and effective pollution abatement strategies.展开更多
Metastable amorphous ferrihydrite(Fh),ubiquitous in redox-dynamic environments,regulates associated trace metal(Cd,As)fate.Nevertheless,how the co-presence of Cd and As influences the phase transformation of Fh and th...Metastable amorphous ferrihydrite(Fh),ubiquitous in redox-dynamic environments,regulates associated trace metal(Cd,As)fate.Nevertheless,how the co-presence of Cd and As influences the phase transformation of Fh and the mobility of coexisting Cd and As remains elusive.Herein,we incubated Fh nanoparticles with Cd/As at pH 6.0 under 25℃ and 75℃ for 60 days.Solution concentrations were monitored,and transformed solids were extracted with P/Ca at pH 4.0/8.0.We showed that aging enhanced Cd and As adsorption in binaryernary systems,with As co-presence significantly promoting Cd sorption.However,75℃aging caused partial Cd and As release after 60 days.The assessment of sorption stability following incubation indicated that Cd and As exhibited distinct behaviors during the extraction by P and Ca.This phenomenon arises from electrostatic interactions between adsorbates and extractant and variations in sorption affinity between Cd and As towards Fh.Elevated temperatures altered the Fh surface structure,enhancing As immobilization but reducing Cd retention.Notably,Cd-As co-presence mutually enhanced release due to ternary complex instability.X-ray powder diffraction(XRD),transmission electron microscopy(TEM),and fourier transform infrared spectroscopy(FTIR)results showed that mixed mineral phases(goethite,hematite,and Fh)were detected at relatively lower Cd and As concentrations.Further extraction experiments revealed that the non-extractable state(structurally incorporated or pore blocked)of Cd and As increased to 42.8%and 89.7%,respectively,at lower Cd-As concentrations.Overall,the aging process induces alterations in Fh surface properties(specific surface area,reactive sites,mixed phases,etc.),diminishing Cd/As stability and facilitating its release with competitive ions.展开更多
This study explores the competitive mechanisms of different types of microplastics(MPs)on pentavalent arsenic(As(Ⅴ))adsorption by magnetic biochar-supported layered double hydroxide composite(MBC@LDH).The effects of ...This study explores the competitive mechanisms of different types of microplastics(MPs)on pentavalent arsenic(As(Ⅴ))adsorption by magnetic biochar-supported layered double hydroxide composite(MBC@LDH).The effects of the solution pH,ionic strength,temperature,material dosage,and MP concentration on As(Ⅴ)adsorption were investigated in co-existing MPs and MBC@LDH systems.Results revealed MPs competitively occupied As(Ⅴ)adsorption sites on MBC@LDH,with varying inhibition efficiencies:polyvinyl chloride(PVC)provided 45.44%of the competitive adsorption,representing a significant reduction in adsorption affinity especially in acidic environments and higher ionic strength.The reduced percentage of adsorption capacity of MBC@LDH for As(Ⅴ)induced by polystyrene(PS)was 35.55%,and that for polyethylene(PE)was also just between PVC and PS,especially in acidic environments and higher ionic strength.Further exploration manifested that the presence of MPs decreased the crystallinity of the CaMgAl LDH in MBC@LDH,which disrupted the surface complexation and hydrogen bonding between MBC-LDH and As.In addition,the strengths of the As–O bonds in MBC@LDH were more significantly reduced by PVC with its entering into the binary system rather than PS and PE,which was ascribable to the strong negative charge and hydrophobic separation properties of PVC.Interestingly,PVC promoted the conversion of As(Ⅴ)to As(Ⅲ)on MBC@LDH but not when PE and PS were added,which might be related to the surface chemical bonding and polarity of the different MPs.This study provides a theoretical reference for MPs'competitive adsorption mechanisms of As on porous materials in aqueous environments.展开更多
Zero-valent iron(ZVI)is widely used in environmental remediation owing to its strong reducing properties.However,passivation deactivation seriously limits the long-term performance.This study explored the passivation ...Zero-valent iron(ZVI)is widely used in environmental remediation owing to its strong reducing properties.However,passivation deactivation seriously limits the long-term performance.This study explored the passivation characteristics of ZVI under common conditions(air,oxygenated water,and pollutants)and elucidated the mechanism of sulfidation depassivation.Results showed that the passivation conditions determined the physicochemical properties of passivated ZVI.Passivation in air forms low-crystalline α-Fe2O3/γ-Fe2O3layers with limited electron transfer capability(ETC).Passivation in oxygenated water leads to the formation of a porous structure dominated byγ-FeOOH,which exhibits a 100-fold increase in specific surface area and enhanced ETC due to the presence of Fe(II)-O.Passivation in Cr(VI)solution forms α-Fe2O3/γ-Fe2O3and Cr-Fe complex layers,which almost lose ETC.Sulfidation effectively removes the passivation layer and forms an FeS layer with excellent ETC;however,its depassivation performance depends on the passivation conditions.Sulfidation of ZVI passivated in air produces highly crystalline FeS with limited thickness.Sulfidation of ZVI passivated in oxygenated water generates low-crystallinity FeS containing iron-oxides(γ-FeOOH and α-Fe2O3),with the smallest internal/external S/Fe molar ratio discrepancy and the strongest ETC.Sulfidation of ZVI passivated in Cr(VI)solution produces low-crystallinity FeS and Fe3S4,with the highest O content(up to 77.6%)and the lowest ETC.Importantly,the Cr(VI)removal ability of passivated and sulfidation-depassivated ZVI is tightly regulated by the passivation conditions and time,and particle size.This paper proposes a sulfidation strategy to address the passivation deactivation of ZVI,thereby promoting its sustainable application in environmental remediation.展开更多
Emerging pollutants—including PFAS,microplastics,antibiotics,and endocrine-disrupting chemicals(EDCs)—pose escalating ecological and health risks while embodying untapped elemental value.Traditional remediation stra...Emerging pollutants—including PFAS,microplastics,antibiotics,and endocrine-disrupting chemicals(EDCs)—pose escalating ecological and health risks while embodying untapped elemental value.Traditional remediation strategies focus on destruction,often overlooking opportunities for resource recovery.In contrast,catalytic upcycling leverages advances in photocatalysis,electrocatalysis,mechanochemistry,and hybrid bio-abiotic systems to selectively convert pollutants into value-added products,aligning with circular economy goals.This review synthesizes overarching catalytic principles—such as C–F and C–C bond activation,ROS selectivity,and redox synergies—that are applicable across pollutant classes.We also contrast pollutant-specific challenges:the chemical inertness of PFAS,the heterogeneity of microplastics,the toxicity and complexity of antibiotic intermediates,and the trace-level persistence of EDCs.Despite these differences,recent breakthroughs demonstrate promising upcycling pathways:PFAS into fluorochemicals,microplastics into olefins and graphitic materials,antibiotics into hydrogen and organic acids,and EDCs into polymeric and pharmaceutical precursors.We further highlight emerging techno-economic and life-cycle assessments,showing that upcycling can reduce CO2emissions by up to 80%and generate substantial economic returns.By reframing pollutants as chemical feedstocks,this review outlines a transformative strategy for pollution control,resource recovery,and sustainable chemical production.展开更多
Arsenic contamination represents a global environmental challenge,with trivalent arsenic(As(III))posing significantly higher risks than pentavalent arsenic(As(V)).Compared to conventional arsenic removal approaches,mi...Arsenic contamination represents a global environmental challenge,with trivalent arsenic(As(III))posing significantly higher risks than pentavalent arsenic(As(V)).Compared to conventional arsenic removal approaches,mineral immobilization technology demonstrates superior efficiency,cost-effectiveness,and environmental compatibility by sequestering arsenic within stable crystalline structures.However,since arsenic in most arsenic-containing minerals exists in the pentavalent form,the arsenic mineral immobilization method requires pre-oxidation of As(III)to As(V),which compromises efficiency and increases operational costs.Tooeleite(Fe6(AsO3)4(SO4)(OH)4・4H2O),as the sole naturally occurring mineral capable of directly immobilizing As(III)without the pre-oxidation,with potential applications for arsenic removal from wastewater.However,there is a lack of comprehensive reviews that systematically evaluate the influencing factors and mechanisms of tooeleite mineralization in arsenic removal.This work systematically reviews the geochemical origin,crystal structure,thermodynamic stability,and environmental persistence of tooeleite.And the critical regulatory factors governing both biotic and abiotic synthesis pathways,including pH conditions,Fe/As/S ratios and microbial interactions,are elucidated.Evaluating the arsenic removal efficiency,limitations,and mineralization pathways of chemical versus biological synthesis approaches,Finally,future research potentials are proposed to advance the engineering applications of tooeleite,thereby providing theoretical foundations and technical references for targeted arsenic pollution remediation.展开更多
摘要Microplastics(MPs)are ubiquitous and pose an environmental risk.This review examined MP pollution in terrestrial ecosystems from a myriad of poorly understood sources.Knowledge regarding the occurrence sources,migration behaviors,ecotoxicology,absorption mechanisms,and effects of MPs has also been fully summarized.Microplastics interact with contaminants,such as antibiotics,pesticides,heavy metals,etc.,and may act as vectors for contaminant transfer in terrestrial ecosystems.The transportation and retention of MPs in soil are governed by interactions among their inherent properties,such as size,shape,surface charge,and density.Interestingly,MP migration into soil is lacking research.The MPs and nanoplastics were also found in edible fruits and vegetables.The MP contamination in soil affects ecosystems,causing soil structure changes,fertility reduction,and pollutant leaching into groundwater.The MP concentration lies in the range of 43-2443 and 40-43000 items kg-1in agricultural and urban soils,respectively.This review provides a comprehensive roadmap for future research and a framework for soil MP risk assessment.Future studies on the uptake,accumulation,and translocation of MPs and their associated toxins by plants are essential for evaluating their risks to food security and human health.Research on MPs in terrestrial habitats lacks comprehensive data on their long-term persistence,degradation pathways,and interactions with soil components under varying environmental conditions.Additionally,limited understanding exists regarding MP impacts on soil biodiversity,pollutant mobility,and plant uptake,highlighting the need for innovative detection methods and effective pollution abatement strategies.
基金supported by Yuelushan Laboratory Talent Program(No.2024RC2033)the National Natural Science Foundation of China(Nos.42407530 and 42207043)+2 种基金the Natural Science Foundation of Hunan Province(No.2023JJ40328)China Postdoctoral Science Foundation(No.2022M721110)the Agricultural Science and Technology Innovation Fund of Hunan Province(No.2024CX106)。
摘要Metastable amorphous ferrihydrite(Fh),ubiquitous in redox-dynamic environments,regulates associated trace metal(Cd,As)fate.Nevertheless,how the co-presence of Cd and As influences the phase transformation of Fh and the mobility of coexisting Cd and As remains elusive.Herein,we incubated Fh nanoparticles with Cd/As at pH 6.0 under 25℃ and 75℃ for 60 days.Solution concentrations were monitored,and transformed solids were extracted with P/Ca at pH 4.0/8.0.We showed that aging enhanced Cd and As adsorption in binaryernary systems,with As co-presence significantly promoting Cd sorption.However,75℃aging caused partial Cd and As release after 60 days.The assessment of sorption stability following incubation indicated that Cd and As exhibited distinct behaviors during the extraction by P and Ca.This phenomenon arises from electrostatic interactions between adsorbates and extractant and variations in sorption affinity between Cd and As towards Fh.Elevated temperatures altered the Fh surface structure,enhancing As immobilization but reducing Cd retention.Notably,Cd-As co-presence mutually enhanced release due to ternary complex instability.X-ray powder diffraction(XRD),transmission electron microscopy(TEM),and fourier transform infrared spectroscopy(FTIR)results showed that mixed mineral phases(goethite,hematite,and Fh)were detected at relatively lower Cd and As concentrations.Further extraction experiments revealed that the non-extractable state(structurally incorporated or pore blocked)of Cd and As increased to 42.8%and 89.7%,respectively,at lower Cd-As concentrations.Overall,the aging process induces alterations in Fh surface properties(specific surface area,reactive sites,mixed phases,etc.),diminishing Cd/As stability and facilitating its release with competitive ions.
基金supported by the National Natural Science Foundation of China(No.42377257)。
摘要This study explores the competitive mechanisms of different types of microplastics(MPs)on pentavalent arsenic(As(Ⅴ))adsorption by magnetic biochar-supported layered double hydroxide composite(MBC@LDH).The effects of the solution pH,ionic strength,temperature,material dosage,and MP concentration on As(Ⅴ)adsorption were investigated in co-existing MPs and MBC@LDH systems.Results revealed MPs competitively occupied As(Ⅴ)adsorption sites on MBC@LDH,with varying inhibition efficiencies:polyvinyl chloride(PVC)provided 45.44%of the competitive adsorption,representing a significant reduction in adsorption affinity especially in acidic environments and higher ionic strength.The reduced percentage of adsorption capacity of MBC@LDH for As(Ⅴ)induced by polystyrene(PS)was 35.55%,and that for polyethylene(PE)was also just between PVC and PS,especially in acidic environments and higher ionic strength.Further exploration manifested that the presence of MPs decreased the crystallinity of the CaMgAl LDH in MBC@LDH,which disrupted the surface complexation and hydrogen bonding between MBC-LDH and As.In addition,the strengths of the As–O bonds in MBC@LDH were more significantly reduced by PVC with its entering into the binary system rather than PS and PE,which was ascribable to the strong negative charge and hydrophobic separation properties of PVC.Interestingly,PVC promoted the conversion of As(Ⅴ)to As(Ⅲ)on MBC@LDH but not when PE and PS were added,which might be related to the surface chemical bonding and polarity of the different MPs.This study provides a theoretical reference for MPs'competitive adsorption mechanisms of As on porous materials in aqueous environments.
基金supported by the National Key and R&D Program of China(No.2024YFC3713004)the China Petroleum and Chemical Corp(No.324036).
摘要Zero-valent iron(ZVI)is widely used in environmental remediation owing to its strong reducing properties.However,passivation deactivation seriously limits the long-term performance.This study explored the passivation characteristics of ZVI under common conditions(air,oxygenated water,and pollutants)and elucidated the mechanism of sulfidation depassivation.Results showed that the passivation conditions determined the physicochemical properties of passivated ZVI.Passivation in air forms low-crystalline α-Fe2O3/γ-Fe2O3layers with limited electron transfer capability(ETC).Passivation in oxygenated water leads to the formation of a porous structure dominated byγ-FeOOH,which exhibits a 100-fold increase in specific surface area and enhanced ETC due to the presence of Fe(II)-O.Passivation in Cr(VI)solution forms α-Fe2O3/γ-Fe2O3and Cr-Fe complex layers,which almost lose ETC.Sulfidation effectively removes the passivation layer and forms an FeS layer with excellent ETC;however,its depassivation performance depends on the passivation conditions.Sulfidation of ZVI passivated in air produces highly crystalline FeS with limited thickness.Sulfidation of ZVI passivated in oxygenated water generates low-crystallinity FeS containing iron-oxides(γ-FeOOH and α-Fe2O3),with the smallest internal/external S/Fe molar ratio discrepancy and the strongest ETC.Sulfidation of ZVI passivated in Cr(VI)solution produces low-crystallinity FeS and Fe3S4,with the highest O content(up to 77.6%)and the lowest ETC.Importantly,the Cr(VI)removal ability of passivated and sulfidation-depassivated ZVI is tightly regulated by the passivation conditions and time,and particle size.This paper proposes a sulfidation strategy to address the passivation deactivation of ZVI,thereby promoting its sustainable application in environmental remediation.
基金supported by the Natural Science Foundation of China(Nos.22225604,U24A20518,and 22422605)the Tianjin Commission of Science and Technology as key critical technologies R&D projects(No.23YFZCSN00010)+3 种基金the Frontiers Science Center for New Organic Matter(No.63181206)Young Scientific and Technological Talents(Level Two)in Tianjin(No.QN20230206)the Fundamental Research Funds for the Central Universities,Nankai University(Nos.63231195 and 63253207)Haihe Laboratory of Sustainable Chemical Transformationsfunded by the Shanghai Tongji Gao Tingyao Environmental Science&Technology Development Foundation.
摘要Emerging pollutants—including PFAS,microplastics,antibiotics,and endocrine-disrupting chemicals(EDCs)—pose escalating ecological and health risks while embodying untapped elemental value.Traditional remediation strategies focus on destruction,often overlooking opportunities for resource recovery.In contrast,catalytic upcycling leverages advances in photocatalysis,electrocatalysis,mechanochemistry,and hybrid bio-abiotic systems to selectively convert pollutants into value-added products,aligning with circular economy goals.This review synthesizes overarching catalytic principles—such as C–F and C–C bond activation,ROS selectivity,and redox synergies—that are applicable across pollutant classes.We also contrast pollutant-specific challenges:the chemical inertness of PFAS,the heterogeneity of microplastics,the toxicity and complexity of antibiotic intermediates,and the trace-level persistence of EDCs.Despite these differences,recent breakthroughs demonstrate promising upcycling pathways:PFAS into fluorochemicals,microplastics into olefins and graphitic materials,antibiotics into hydrogen and organic acids,and EDCs into polymeric and pharmaceutical precursors.We further highlight emerging techno-economic and life-cycle assessments,showing that upcycling can reduce CO2emissions by up to 80%and generate substantial economic returns.By reframing pollutants as chemical feedstocks,this review outlines a transformative strategy for pollution control,resource recovery,and sustainable chemical production.
基金supported by the National Key R&D Program of China(No.2022YFD1700101)the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.52121004).
摘要Arsenic contamination represents a global environmental challenge,with trivalent arsenic(As(III))posing significantly higher risks than pentavalent arsenic(As(V)).Compared to conventional arsenic removal approaches,mineral immobilization technology demonstrates superior efficiency,cost-effectiveness,and environmental compatibility by sequestering arsenic within stable crystalline structures.However,since arsenic in most arsenic-containing minerals exists in the pentavalent form,the arsenic mineral immobilization method requires pre-oxidation of As(III)to As(V),which compromises efficiency and increases operational costs.Tooeleite(Fe6(AsO3)4(SO4)(OH)4・4H2O),as the sole naturally occurring mineral capable of directly immobilizing As(III)without the pre-oxidation,with potential applications for arsenic removal from wastewater.However,there is a lack of comprehensive reviews that systematically evaluate the influencing factors and mechanisms of tooeleite mineralization in arsenic removal.This work systematically reviews the geochemical origin,crystal structure,thermodynamic stability,and environmental persistence of tooeleite.And the critical regulatory factors governing both biotic and abiotic synthesis pathways,including pH conditions,Fe/As/S ratios and microbial interactions,are elucidated.Evaluating the arsenic removal efficiency,limitations,and mineralization pathways of chemical versus biological synthesis approaches,Finally,future research potentials are proposed to advance the engineering applications of tooeleite,thereby providing theoretical foundations and technical references for targeted arsenic pollution remediation.