This study addresses the synthesis of nanoscale zero-valent iron(n ZVI) in the presence of natural bentonite(B-n ZVI) using green tea extract. The natural bentonite and B-n ZVI were then applied for the removal of pho...This study addresses the synthesis of nanoscale zero-valent iron(n ZVI) in the presence of natural bentonite(B-n ZVI) using green tea extract. The natural bentonite and B-n ZVI were then applied for the removal of phosphorus from aqueous solutions at various concentrations, p H levels and contact time. The desorption of phosphorus(P) from adsorbents was done immediately after sorption at the maximum initial concentration using the successive dilution method. The characterization of FTIR, SEM, and XRD indicated that n ZVI was successfully loaded to the surface of natural bentonite. The sorption of phosphorus on B-n ZVI was observed to be p H-dependent, with maximum phosphorus removal occurring at the p H range of 2 to 5. The results demonstrate that the maximum sorption capacities of natural bentonite and B-n ZVI were 4.61 and 27.63 mg·g^(-1), respectively.Langmuir, Freundlich, and Redlich–Peterson models properly described the sorption isotherm data. For either adsorbent, desorption isotherms did not coincide with their corresponding sorption isotherms, suggesting the occurrence of irreversibility and hysteresis. The average percentages of retained phosphorus released from natural bentonite and B-n ZVI were 80% and 9%, respectively. The results indicated that sorption kinetics was best described by the pseudo-second-order model. The present study suggests that B-n ZVI could be used as a suitable adsorbent for the removal of phosphorus from aqueous solutions.展开更多
The present research investigated a novel route for the synthesis of nanoparticle zero-valent iron(NZVI)utilizing an aqueous extract of green tea waste as a reductant with ferric chloride.Also,the supported nanopartic...The present research investigated a novel route for the synthesis of nanoparticle zero-valent iron(NZVI)utilizing an aqueous extract of green tea waste as a reductant with ferric chloride.Also,the supported nanoparticle zerovalent iron was synthesized using natural silty clay as a support material(SC-NZVI).The NZVI and SC-NZVI were characterized by infrared spectroscopy(FTIR),scanning electron microscope(SEM),X-ray diffraction(XRD),Brunauer–Emmett–Teller(BET),and zeta potential(ζ).The interpretation of the results demonstrated that the polyphenol and other antioxidants in green tea waste can be used as reduction and capping agents in NZVI synthesis,with silty clay an adequate support.Additionally,the experiments were carried out to explore phenol adsorption by NZVI and SC-NZVI.To determine the optimum conditions,the impact of diverse experimental factors(i.e.,initial pH,adsorbent dose,temperature,and concentration of phenol)was studied.Langmuir,Freundlich,and Tempkin isotherms were used as representatives of adsorption equilibrium.The obtained results indicated that the adsorption processes for both NZVI and SC-NZVI well fitted by the Freundlich isotherm model.The appropriateness of pseudofirstorder and pseudosecondorder kinetics was investigated.The experimental kinetics data were good explained by the second-order model.The thermodynamic parameters(ΔH0,ΔS0,andΔG0)for NZVI and SC-NZVI were determined.The maximum removal rates of phenol at optimum conditions,when adsorbed onto NZVI and SC-NZVI,were found to be 94.8%and 90.1%,respectively.展开更多
Diclofenac(DCF)is one of the most frequently detected pharmaceuticals in groundwater,posing a great threat to the environment and human health due to its toxicity.To mitigate the DCF contamination,experiments on DCF d...Diclofenac(DCF)is one of the most frequently detected pharmaceuticals in groundwater,posing a great threat to the environment and human health due to its toxicity.To mitigate the DCF contamination,experiments on DCF degradation by the combined process of zero-valent iron nanoparticles(nZVI)and nano calcium peroxide(nCaO_(2))were performed.A batch experiment was conducted to examine the influence of the adding dosages of both nZVI and nCaO_(2)nanoparticles and pH value on the DCF removal.In the meantime,the continuous-flow experiment was done to explore the sustainability of the DCF degradation by jointly adding nZVI/nCaO_(2)nanoparticles in the reaction system.The results show that the nZVI/nCaO_(2)can effectively remove the DCF in the batch test with only 0.05 g/L nZVI and 0.2 g/L nCaO_(2)added,resulting in a removal rate of greater than 90%in a 2-hour reaction with an initial pH of 5.The degradation rate of DCF was positively correlated with the dosage of nCaO_(2),and negatively correlated with both nZVI dosage and the initial pH value.The order of significance of the three factors is identified as pH value>nZVI dosage>nCaO_(2)dosage.In the continuous-flow reaction system,the DCF removal rates remained above 75%within 150 minutes at the pH of 5,with the applied dosages of 0.5 g/L for nZVI and 1.0 g/L for nCaO_(2).These results provide a theoretical basis for the nZVI/nCaO_(2)application to remove DCF in groundwater.展开更多
In this study, novel core-shell SiO<sub>2</sub>-coated iron nanoparticles (SiO<sub>2</sub>-nZVI) were synthesized using a one-step Stoeber method. The Malachite green degradation abilities of t...In this study, novel core-shell SiO<sub>2</sub>-coated iron nanoparticles (SiO<sub>2</sub>-nZVI) were synthesized using a one-step Stoeber method. The Malachite green degradation abilities of the nanoparticles were investigated. The effects of ethanol/distilled water volume ratio, presence and absence of PEG, tetraethyl orthosilicate (TEOS) dosage, and hydrolysis time used in the nanoparticles preparation process were investigated. The results indicated that the SiO<sub>2</sub>-coated iron nanoparticles had the highest reduction activity when the particles synthesized with ethanol/H<sub>2</sub>O ratio of 2:1, PEG of 0.15 ml, TEOS of 0.5 ml and the reaction time was 4 h. The SiO<sub>2</sub>-nZVI nanoparticles were characterized using Transmission Electron Microscopy (TEM), Energy Dispersive Spectrometry (EDS) and powder X-Ray Diffraction (XRD). The results showed that the average particles diameter of the SiO<sub>2</sub>-nZVI was 20 - 30 nm. The thickness of the outside SiO<sub>2</sub> film is consistent and approximately 10 nm. The results indicated that the nanoparticles coated completely with a transparent SiO<sub>2</sub>-film. Such nanoparticles could have wide applications in dye decolorization.展开更多
The addition of nano zero-valent iron(nZVI)is a promising technology for the in situ remediation of soil.Unfortunately,the mobility and,consequently,the reactivity of nZVI particles in contaminated areas decrease due ...The addition of nano zero-valent iron(nZVI)is a promising technology for the in situ remediation of soil.Unfortunately,the mobility and,consequently,the reactivity of nZVI particles in contaminated areas decrease due to their rapid aggregation.In this study,we determined how nZVI particles can be stabilized using different types of biochar(BC)as a support(BC@nZVI).In addition,we investigated the transport behavior of the synthesized BC@nZVI particles in a column filled with porous media and their effectiveness in the removal of BDE209(decabromodiphenyl ether)from soil.The characterization results of N2 Brunauer-Emmett-Teller(BET)surface area analyses,scanning electron microscopy(SEM),X-ray diffraction(XRD)and Fourier transform infrared spectroscopy(FTIR)indicated that nZVI was successfully loaded into the BC.The sedimentation test results and the experimental breakthrough curves indicated that all of the BC@nZVI composites manifested better stability and mobility than did the bare-nZVI particles,and the transport capacity of the particles increased with increasing flow velocity and porous medium size.Furthermore,the maximum concentrations of the column effluent for bagasse-BC@nZVI(B-BC@nZVI)were 19%,37%and 48%higher than those for rice straw-BC@nZVI(R-BC@nZVI),wood chips-BC@nZVI(W-BC@nZVI)and corn stalks-BC@nZVI(C-BC@nZVI),respectively.A similar order was found for the removal and debromination efficiency of decabromodiphenyl ether(BDE209)by the aforementioned particles.Overall,the attachment of nZVI particles to BC significantly increased the reactivity,stability and mobility of B-BC@nZVI yielded,and nZVI the best performance.展开更多
Arsenic(As)and antimony(Sb)are usually coexistent in mine wastes and pose a great threat to human health.The As immobilization by nano zero-valent iron(n ZVI)is promising,however,the stabilization for co-occurring As ...Arsenic(As)and antimony(Sb)are usually coexistent in mine wastes and pose a great threat to human health.The As immobilization by nano zero-valent iron(n ZVI)is promising,however,the stabilization for co-occurring As and Sb is not known.Herein,the immobilization and transformation of As and Sb in n ZVI-treated sediments were evaluated using complementary leaching experiments and characterization techniques.Raw sediment samples from a gold-antimony deposit revealed the co-existence of ultrahigh As and Sb at 50.3 and 14.9 g/kg,respectively.Leaching results show that As was more efficiently stabilized by n ZVI than Sb,which was primarily due to the soluble fraction that was readily absorbed by n ZVI of As was higher.As the n ZVI treatment proceeds,the oxidation and reduction of As and Sb occur simultaneously as evidenced by XPS analysis.The primary oxidant,hydroxyl radicals,was detected by EPR studies,proving the occurrence of n ZVI induced Fenton reaction.This study sheds light on differences in the interaction and immobilization of n ZVI with Sb and As in co-contaminated sediments.展开更多
The aim of this work is to optimize iron nanoparticle production in stirred tank reactors equipped with two classical impellers:Rushton and four-pitched blade turbines,which are largely used in batch industrial synthe...The aim of this work is to optimize iron nanoparticle production in stirred tank reactors equipped with two classical impellers:Rushton and four-pitched blade turbines,which are largely used in batch industrial synthesis and efficient scale-up.The main operative parameters of nanoparticle synthesis are the precursor initial concentration,reducing agent/precursor molar ratio,impeller-tank clearance,and impeller rotational velocity.These parameters were varied during the synthesis to find the optimal operating values based on the Fe(0)(%)production,zeta potential,particle size distribution,and powder X-ray diffraction pattern obtained.We found that the optimal operating conditions for nanoparticle production were an impeller velocity of 1500 rpm,initial iron precursor concentration of 20 mM,molar ratio of reducing agent to iron precursor of 3 mol/mol,and impeller clearance of 0.25 and 0.4 times the vessel diameter for Rushton and four-pitched blade impellers,respectively.Setting these conditions achieved a total conversion of 0.94-0.98 and yielded a product with a unimodal size distribution and average diameters in the range 30-50 nm.The computational fluid dynamics results agreed with the expectations,and the obtained mixing Damkohler numbers show that the process is mixed controlled.展开更多
The earthworm-based vermiremediation facilitated with benign chemicals such as nano zero-valent iron(nZVI)is a promising approach for the remediation of a variety of soil contaminants including cyanotoxins.As themost ...The earthworm-based vermiremediation facilitated with benign chemicals such as nano zero-valent iron(nZVI)is a promising approach for the remediation of a variety of soil contaminants including cyanotoxins.As themost toxic cyanotoxin,microcystin-LR(MC-LR)enter soil via runoff,irrigated surface water and sewage,and the application of cyanobacterial biofertilizers as part of the sustainable agricultural practice.Earthworms in such remediation systems must sustain the potential risk from both nZVI and MC-LR.In the present study,earthworms(Eisenia fetida)were exposed up to 14 days to MC-LR and nZVI(individually and inmixture),and the toxicity was investigated at both the organismal andmetabolic levels,including growth,tissue damage,oxidative stress,metabolic response and gut microbiota.Results showed that co-exposure of MC-LR and nZVI is less potent to earthworms than that of separate exposure.Histological observations in the co-exposure group revealed only minor epidermal brokenness,and KEGG enrichment analysis showed that co-exposure induced earthworms to regulate glutathione biosynthesis for detoxification and reduced adverse effects from MC-LR.The combined use of nZVI promoted the growth and reproduction of soil and earthworm gut bacteria(e.g.,Sphingobacterium and Acinetobacter)responsible for the degradation of MC-LR,whichmight explain the observed antagonism between nZVI and MC-LR in earthworm microcosm.Our study suggests the beneficial use of nZVI to detoxify pollutants in earthworm-based vermiremediation systems where freshwater containing cyanobacterial blooms is frequently used to irrigate soil and supply water for the growth and metabolism of earthworms.展开更多
Nano zero-valent iron(nZVI)is a promising phosphate adsorbent for advanced phosphate removal.However,the rapid passivation of nZVI and the low activity of adsorption sites seriously limit its phosphate removal perform...Nano zero-valent iron(nZVI)is a promising phosphate adsorbent for advanced phosphate removal.However,the rapid passivation of nZVI and the low activity of adsorption sites seriously limit its phosphate removal performance,accounting for its inapplicability to meet the emission criteria of 0.1 mg P/L phosphate.In this study,we report that the oxalate modification can inhibit the passivation of nZVI and alter the multi-stage phosphate adsorption mechanism by changing the adsorption sites.As expected,the stronger antipassivation ability of oxalate modified nZVI(OX-nZVI)strongly favored its phosphate adsorption.Interestingly,the oxalate modification endowed the surface Fe(III)sites with the lowest chemisorption energy and the fastest phosphate adsorption ability than the other adsorption sites,by in situ forming a Fe(III)-phosphate-oxalate ternary complex,therefore enabling an advanced phosphate removal process.At an initial phosphate concentration of 1.00 mg P/L,pH of 6.0 and a dosage of 0.3 g/L of adsorbents,OX-nZVI exhibited faster phosphate removal rate(0.11 g/mg/min)and lower residual phosphate level(0.02 mg P/L)than nZVI(0.055 g/mg/min and 0.19 mg P/L).This study sheds light on the importance of site manipulation in the development of high-performance adsorbents,and offers a facile surface modification strategy to prepare superior iron-basedmaterials for advanced phosphate removal.展开更多
Paddy soil and irrigation water are commonly contaminated with hexavalent chromium[Cr(Ⅵ)]near urban industrial areas,thereby threatening the safety of agricultural products and human health.In this study,we develop a...Paddy soil and irrigation water are commonly contaminated with hexavalent chromium[Cr(Ⅵ)]near urban industrial areas,thereby threatening the safety of agricultural products and human health.In this study,we develop a porous and high specific area bone char(BC)to support nanoscale zero-valent iron(n ZVI)and apply it to remediate Cr(Ⅵ)pollution in water and paddy soil under anaerobic conditions.The batch experiments reveal that BC/n ZVI exhibits a higher removal capacity of 516.7 mg/(g·n ZVI)for Cr(Ⅵ)than n ZVI when normalized to the actual n ZVI content,which is 2.8 times that of n ZVI;moreover,the highest n ZVI utilization is the n ZVI loading of 15%(BC/n ZVI15).The Cr(Ⅵ)removal efficiency of BC/n ZVI15 decreases with increasing p H(4–10).Coexisting ions(phosphate and carbonate)and humic acid can inhibit the removal of Cr(Ⅵ)with BC/n ZVI15.Additionally,BC exhibits a strong advantage in promoting Cr(Ⅵ)removal by n ZVI compared to the widely used biochar and activated carbon.Our results demonstrate that reduction and coprecipitation are the dominant Cr(Ⅵ)removal mechanisms.Furthermore,BC/n ZVI15 shows a significantly higher reduction and removal efficiency as well as a strong anti-interference ability for Cr(Ⅵ)in paddy soil,as compared to n ZVI.These findings provide a new effective material for remediating Cr(Ⅵ)pollution from water and soil.展开更多
文摘This study addresses the synthesis of nanoscale zero-valent iron(n ZVI) in the presence of natural bentonite(B-n ZVI) using green tea extract. The natural bentonite and B-n ZVI were then applied for the removal of phosphorus from aqueous solutions at various concentrations, p H levels and contact time. The desorption of phosphorus(P) from adsorbents was done immediately after sorption at the maximum initial concentration using the successive dilution method. The characterization of FTIR, SEM, and XRD indicated that n ZVI was successfully loaded to the surface of natural bentonite. The sorption of phosphorus on B-n ZVI was observed to be p H-dependent, with maximum phosphorus removal occurring at the p H range of 2 to 5. The results demonstrate that the maximum sorption capacities of natural bentonite and B-n ZVI were 4.61 and 27.63 mg·g^(-1), respectively.Langmuir, Freundlich, and Redlich–Peterson models properly described the sorption isotherm data. For either adsorbent, desorption isotherms did not coincide with their corresponding sorption isotherms, suggesting the occurrence of irreversibility and hysteresis. The average percentages of retained phosphorus released from natural bentonite and B-n ZVI were 80% and 9%, respectively. The results indicated that sorption kinetics was best described by the pseudo-second-order model. The present study suggests that B-n ZVI could be used as a suitable adsorbent for the removal of phosphorus from aqueous solutions.
文摘The present research investigated a novel route for the synthesis of nanoparticle zero-valent iron(NZVI)utilizing an aqueous extract of green tea waste as a reductant with ferric chloride.Also,the supported nanoparticle zerovalent iron was synthesized using natural silty clay as a support material(SC-NZVI).The NZVI and SC-NZVI were characterized by infrared spectroscopy(FTIR),scanning electron microscope(SEM),X-ray diffraction(XRD),Brunauer–Emmett–Teller(BET),and zeta potential(ζ).The interpretation of the results demonstrated that the polyphenol and other antioxidants in green tea waste can be used as reduction and capping agents in NZVI synthesis,with silty clay an adequate support.Additionally,the experiments were carried out to explore phenol adsorption by NZVI and SC-NZVI.To determine the optimum conditions,the impact of diverse experimental factors(i.e.,initial pH,adsorbent dose,temperature,and concentration of phenol)was studied.Langmuir,Freundlich,and Tempkin isotherms were used as representatives of adsorption equilibrium.The obtained results indicated that the adsorption processes for both NZVI and SC-NZVI well fitted by the Freundlich isotherm model.The appropriateness of pseudofirstorder and pseudosecondorder kinetics was investigated.The experimental kinetics data were good explained by the second-order model.The thermodynamic parameters(ΔH0,ΔS0,andΔG0)for NZVI and SC-NZVI were determined.The maximum removal rates of phenol at optimum conditions,when adsorbed onto NZVI and SC-NZVI,were found to be 94.8%and 90.1%,respectively.
基金the National Natural Science Foundation of China(42077176,41601514)Shanghai“Science and Technology Innovation Action Plan”Project(19230742400,19ZR1459300)+1 种基金Shanghai Peak Discipline Project(0200121005/053,2019010202)State Key Laboratory of Petroleum Pollution Control(PPC2016019)。
文摘Diclofenac(DCF)is one of the most frequently detected pharmaceuticals in groundwater,posing a great threat to the environment and human health due to its toxicity.To mitigate the DCF contamination,experiments on DCF degradation by the combined process of zero-valent iron nanoparticles(nZVI)and nano calcium peroxide(nCaO_(2))were performed.A batch experiment was conducted to examine the influence of the adding dosages of both nZVI and nCaO_(2)nanoparticles and pH value on the DCF removal.In the meantime,the continuous-flow experiment was done to explore the sustainability of the DCF degradation by jointly adding nZVI/nCaO_(2)nanoparticles in the reaction system.The results show that the nZVI/nCaO_(2)can effectively remove the DCF in the batch test with only 0.05 g/L nZVI and 0.2 g/L nCaO_(2)added,resulting in a removal rate of greater than 90%in a 2-hour reaction with an initial pH of 5.The degradation rate of DCF was positively correlated with the dosage of nCaO_(2),and negatively correlated with both nZVI dosage and the initial pH value.The order of significance of the three factors is identified as pH value>nZVI dosage>nCaO_(2)dosage.In the continuous-flow reaction system,the DCF removal rates remained above 75%within 150 minutes at the pH of 5,with the applied dosages of 0.5 g/L for nZVI and 1.0 g/L for nCaO_(2).These results provide a theoretical basis for the nZVI/nCaO_(2)application to remove DCF in groundwater.
文摘In this study, novel core-shell SiO<sub>2</sub>-coated iron nanoparticles (SiO<sub>2</sub>-nZVI) were synthesized using a one-step Stoeber method. The Malachite green degradation abilities of the nanoparticles were investigated. The effects of ethanol/distilled water volume ratio, presence and absence of PEG, tetraethyl orthosilicate (TEOS) dosage, and hydrolysis time used in the nanoparticles preparation process were investigated. The results indicated that the SiO<sub>2</sub>-coated iron nanoparticles had the highest reduction activity when the particles synthesized with ethanol/H<sub>2</sub>O ratio of 2:1, PEG of 0.15 ml, TEOS of 0.5 ml and the reaction time was 4 h. The SiO<sub>2</sub>-nZVI nanoparticles were characterized using Transmission Electron Microscopy (TEM), Energy Dispersive Spectrometry (EDS) and powder X-Ray Diffraction (XRD). The results showed that the average particles diameter of the SiO<sub>2</sub>-nZVI was 20 - 30 nm. The thickness of the outside SiO<sub>2</sub> film is consistent and approximately 10 nm. The results indicated that the nanoparticles coated completely with a transparent SiO<sub>2</sub>-film. Such nanoparticles could have wide applications in dye decolorization.
基金The National Key Research and Development Program of China(2018YFC1802802)the Guangdong Technology Research Center for Ecological Management and Remediation of Water Systems(2014B090904077).
文摘The addition of nano zero-valent iron(nZVI)is a promising technology for the in situ remediation of soil.Unfortunately,the mobility and,consequently,the reactivity of nZVI particles in contaminated areas decrease due to their rapid aggregation.In this study,we determined how nZVI particles can be stabilized using different types of biochar(BC)as a support(BC@nZVI).In addition,we investigated the transport behavior of the synthesized BC@nZVI particles in a column filled with porous media and their effectiveness in the removal of BDE209(decabromodiphenyl ether)from soil.The characterization results of N2 Brunauer-Emmett-Teller(BET)surface area analyses,scanning electron microscopy(SEM),X-ray diffraction(XRD)and Fourier transform infrared spectroscopy(FTIR)indicated that nZVI was successfully loaded into the BC.The sedimentation test results and the experimental breakthrough curves indicated that all of the BC@nZVI composites manifested better stability and mobility than did the bare-nZVI particles,and the transport capacity of the particles increased with increasing flow velocity and porous medium size.Furthermore,the maximum concentrations of the column effluent for bagasse-BC@nZVI(B-BC@nZVI)were 19%,37%and 48%higher than those for rice straw-BC@nZVI(R-BC@nZVI),wood chips-BC@nZVI(W-BC@nZVI)and corn stalks-BC@nZVI(C-BC@nZVI),respectively.A similar order was found for the removal and debromination efficiency of decabromodiphenyl ether(BDE209)by the aforementioned particles.Overall,the attachment of nZVI particles to BC significantly increased the reactivity,stability and mobility of B-BC@nZVI yielded,and nZVI the best performance.
基金financial This work was supported by the National Key Basic Research Program of China(No.2020YFC1807800)the National Natural Science Foundation of China(Nos,41877378 and 42077299)the Major Program of Shandong Natural Science Foundation,China(No.ZR2020ZD34)。
文摘Arsenic(As)and antimony(Sb)are usually coexistent in mine wastes and pose a great threat to human health.The As immobilization by nano zero-valent iron(n ZVI)is promising,however,the stabilization for co-occurring As and Sb is not known.Herein,the immobilization and transformation of As and Sb in n ZVI-treated sediments were evaluated using complementary leaching experiments and characterization techniques.Raw sediment samples from a gold-antimony deposit revealed the co-existence of ultrahigh As and Sb at 50.3 and 14.9 g/kg,respectively.Leaching results show that As was more efficiently stabilized by n ZVI than Sb,which was primarily due to the soluble fraction that was readily absorbed by n ZVI of As was higher.As the n ZVI treatment proceeds,the oxidation and reduction of As and Sb occur simultaneously as evidenced by XPS analysis.The primary oxidant,hydroxyl radicals,was detected by EPR studies,proving the occurrence of n ZVI induced Fenton reaction.This study sheds light on differences in the interaction and immobilization of n ZVI with Sb and As in co-contaminated sediments.
文摘The aim of this work is to optimize iron nanoparticle production in stirred tank reactors equipped with two classical impellers:Rushton and four-pitched blade turbines,which are largely used in batch industrial synthesis and efficient scale-up.The main operative parameters of nanoparticle synthesis are the precursor initial concentration,reducing agent/precursor molar ratio,impeller-tank clearance,and impeller rotational velocity.These parameters were varied during the synthesis to find the optimal operating values based on the Fe(0)(%)production,zeta potential,particle size distribution,and powder X-ray diffraction pattern obtained.We found that the optimal operating conditions for nanoparticle production were an impeller velocity of 1500 rpm,initial iron precursor concentration of 20 mM,molar ratio of reducing agent to iron precursor of 3 mol/mol,and impeller clearance of 0.25 and 0.4 times the vessel diameter for Rushton and four-pitched blade impellers,respectively.Setting these conditions achieved a total conversion of 0.94-0.98 and yielded a product with a unimodal size distribution and average diameters in the range 30-50 nm.The computational fluid dynamics results agreed with the expectations,and the obtained mixing Damkohler numbers show that the process is mixed controlled.
基金supported by the National Natural Science Foundation of China(No.21777139)the National Key Research and Development Program of China(No.2017YFA0207003).
文摘The earthworm-based vermiremediation facilitated with benign chemicals such as nano zero-valent iron(nZVI)is a promising approach for the remediation of a variety of soil contaminants including cyanotoxins.As themost toxic cyanotoxin,microcystin-LR(MC-LR)enter soil via runoff,irrigated surface water and sewage,and the application of cyanobacterial biofertilizers as part of the sustainable agricultural practice.Earthworms in such remediation systems must sustain the potential risk from both nZVI and MC-LR.In the present study,earthworms(Eisenia fetida)were exposed up to 14 days to MC-LR and nZVI(individually and inmixture),and the toxicity was investigated at both the organismal andmetabolic levels,including growth,tissue damage,oxidative stress,metabolic response and gut microbiota.Results showed that co-exposure of MC-LR and nZVI is less potent to earthworms than that of separate exposure.Histological observations in the co-exposure group revealed only minor epidermal brokenness,and KEGG enrichment analysis showed that co-exposure induced earthworms to regulate glutathione biosynthesis for detoxification and reduced adverse effects from MC-LR.The combined use of nZVI promoted the growth and reproduction of soil and earthworm gut bacteria(e.g.,Sphingobacterium and Acinetobacter)responsible for the degradation of MC-LR,whichmight explain the observed antagonism between nZVI and MC-LR in earthworm microcosm.Our study suggests the beneficial use of nZVI to detoxify pollutants in earthworm-based vermiremediation systems where freshwater containing cyanobacterial blooms is frequently used to irrigate soil and supply water for the growth and metabolism of earthworms.
基金supported by the National Key Research and Development Program of China(Nos.2022YFA1205602,and 2023YFC3707801)the National Natural Science Foundation of China(Nos.U22A20402,22376073,21936003 and 22306119)China Postdoctoral Science Foundation(No.2023T160419).
文摘Nano zero-valent iron(nZVI)is a promising phosphate adsorbent for advanced phosphate removal.However,the rapid passivation of nZVI and the low activity of adsorption sites seriously limit its phosphate removal performance,accounting for its inapplicability to meet the emission criteria of 0.1 mg P/L phosphate.In this study,we report that the oxalate modification can inhibit the passivation of nZVI and alter the multi-stage phosphate adsorption mechanism by changing the adsorption sites.As expected,the stronger antipassivation ability of oxalate modified nZVI(OX-nZVI)strongly favored its phosphate adsorption.Interestingly,the oxalate modification endowed the surface Fe(III)sites with the lowest chemisorption energy and the fastest phosphate adsorption ability than the other adsorption sites,by in situ forming a Fe(III)-phosphate-oxalate ternary complex,therefore enabling an advanced phosphate removal process.At an initial phosphate concentration of 1.00 mg P/L,pH of 6.0 and a dosage of 0.3 g/L of adsorbents,OX-nZVI exhibited faster phosphate removal rate(0.11 g/mg/min)and lower residual phosphate level(0.02 mg P/L)than nZVI(0.055 g/mg/min and 0.19 mg P/L).This study sheds light on the importance of site manipulation in the development of high-performance adsorbents,and offers a facile surface modification strategy to prepare superior iron-basedmaterials for advanced phosphate removal.
基金financially supported by the National Natural Science Foundation of China(Nos.21876161,42077301,41420104007)the National Key Research and Development Project of China(No.2018YFF0213403)+1 种基金the Guangdong Academy of Sciences'Project(Nos.2019GDASYL-0102006,2019GDASYL-0301002,2018GDASCX-0501)the Research Fund of China Geological Survey(DD20190703)。
文摘Paddy soil and irrigation water are commonly contaminated with hexavalent chromium[Cr(Ⅵ)]near urban industrial areas,thereby threatening the safety of agricultural products and human health.In this study,we develop a porous and high specific area bone char(BC)to support nanoscale zero-valent iron(n ZVI)and apply it to remediate Cr(Ⅵ)pollution in water and paddy soil under anaerobic conditions.The batch experiments reveal that BC/n ZVI exhibits a higher removal capacity of 516.7 mg/(g·n ZVI)for Cr(Ⅵ)than n ZVI when normalized to the actual n ZVI content,which is 2.8 times that of n ZVI;moreover,the highest n ZVI utilization is the n ZVI loading of 15%(BC/n ZVI15).The Cr(Ⅵ)removal efficiency of BC/n ZVI15 decreases with increasing p H(4–10).Coexisting ions(phosphate and carbonate)and humic acid can inhibit the removal of Cr(Ⅵ)with BC/n ZVI15.Additionally,BC exhibits a strong advantage in promoting Cr(Ⅵ)removal by n ZVI compared to the widely used biochar and activated carbon.Our results demonstrate that reduction and coprecipitation are the dominant Cr(Ⅵ)removal mechanisms.Furthermore,BC/n ZVI15 shows a significantly higher reduction and removal efficiency as well as a strong anti-interference ability for Cr(Ⅵ)in paddy soil,as compared to n ZVI.These findings provide a new effective material for remediating Cr(Ⅵ)pollution from water and soil.
