Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing e...Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing effluent and recycling of surfactant solutions.In this study,a molecular imprinting technique was applied to selectively sorb polybrominated diphenyl ethers(PBDEs)in soil washing effluent.The novel molecular imprinted polymers(MIPs)using different template molecules were synthesized by precipitation polymerization.Adsorption behaviors andmechanisms ofMIPs were studied through experiments and theoretical calculations.The results show that 4-bromo-4'-hydroxybiphenyl and toluene can be effective imprinting molecule for MIPs synthesis.The maximal adsorption capacity of selected dummy molecular imprinted polymer(D1-MIP)was 1032.36μmol/g,and that of part molecular imprinted polymer(P-MIP)was 981.13μmol/g.Their imprinting factors in 5 PBDEs adsorption ranged from 2.13 to 5.88,the recovery percentage of Triton X-100 can reach 99.09%,confirming the feasibility of reusing surfactant.Various PBDEs could be removed by MIPs,and Quantitative Structure Property Relationship analysis revealed that PBDEs’molecular volume,planarity,polarity,and hydrophobicity have major influences on their adsorption performance.DFT calculation revealed that Van derWaals force and hydrogen bonding played important roles during selective adsorption.These results can provide effective theoretical guidance for surfactant enhanced soil elution in practical engineering applications.展开更多
Polycyclic aromatic hydrocarbons(PAHs), typical representatives of the persistent organic pollutants(POPs), have become ubiquitous in the environment.In this study, a novel microbial consortium QY1 that performed outs...Polycyclic aromatic hydrocarbons(PAHs), typical representatives of the persistent organic pollutants(POPs), have become ubiquitous in the environment.In this study, a novel microbial consortium QY1 that performed outstanding PAHs-degrading capacity has been enriched.The degradation characteristics of single and mixed PAHs treated with QY1 were studied, and the effect of biochar on biodegradation of mixed PAHs and the potential of biochar in PAHs-heavy metal combined pollution bioremediation were also investigated.Results showed that, in single substrate system, QY1 degraded 94.5% of 500 mg/L phenanthrene(PHE) and 17.8% of 10 mg/L pyrene(PYR) after 7 days, while in PHE-PYR mixture system, the biodegradation efficiencies of PHE(500 mg/L) and PYR(10 mg/L) reached 94.0%and 96.2%, respectively, since PHE served as co-metabolic substrate to have significantly improved PYR biodegradation.Notably, with the cooperation of biochar, the biodegradations of PHE and PYR were greatly accelerated.Further, biochar could reduce the adverse impact of heavy metals(Cd^(2+), Cu^(2+), Cr_(2)O_(7)^(2-)) on PYR biodegradation remarkably.The sequencing analysis revealed that Methylobacterium, Burkholderia and Stenotrophomonas were the dominant genera of QY1 in almost all treatments, indicating that these genera might play key roles in PAHs biodegradation.Overall, this study provided new insights into the efficient bioremediation of PAHs-contaminated site.展开更多
The degradation of 2,2′,4,4′-tetrabromodiphenyl ether(BDE-47) by Pycnoporus sanguineus was investigated in order to explore the impact of the heavy metal Cu2+ on BDE-47 decomposition and the subsequent formation of ...The degradation of 2,2′,4,4′-tetrabromodiphenyl ether(BDE-47) by Pycnoporus sanguineus was investigated in order to explore the impact of the heavy metal Cu2+ on BDE-47 decomposition and the subsequent formation of metabolites, as well as to further elucidate the degradation mechanism of BDE-47. An increase in degradation rate from 18.63% to49.76% in the first four days and its stabilization at(51.26 ± 0.08)% in the following days of BDE-47 incubation were observed. The presence of Cu2+ at 1 and 2 mg/L was found to promote the degradation rate to 56.41% and 60.79%, respectively, whereas higher level of Cu2+(≥ 5 mg/L) inhibited the removal of BDE-47. The similar concentration effects of Cu2+ was also found on contents of fungal protein and amounts of metabolites. Both intracellular and extracellular enzymes played certain roles in BDE-47 transportation with the best degradation rate at 27.90% and 27.67% on the fourth and third day, individually. During the degradation of BDE-47, four types of hydroxylated polybrominated diphenyl ethers(OH-PBDEs), i.e., 6′-OH-BDE-47, 5′-OH-BDE-47, 4′-OH-BDE-17, 2′-OH-BDE-28, and two bromophenols, i.e., 2,4-DBP and 4-BP were detected and considered as degradation products. These metabolites were further removed by P. sanguineus at rates of 22.42%,23.01%, 27.04%, 27.96%, 64.21%, and 40.62%, respectively.展开更多
Schwertmannite is an amorphous iron(III)-oxyhydroxysulfate that forms in acid mine drainage(AMD) environments. The characteristic of high heavy metal adsorption capability makes schwertmannite a potentially useful, en...Schwertmannite is an amorphous iron(III)-oxyhydroxysulfate that forms in acid mine drainage(AMD) environments. The characteristic of high heavy metal adsorption capability makes schwertmannite a potentially useful, environmentally friendly material in wastewater treatment. Unstable schwertmannite is prone to recrystallization.Understanding the mechanisms that induce schwertmannite labilization and affect its capacity to remove heavy metals are of great environmental and geochemical significance.Thiocyanate(SCNˉ) is a hazardous pseudohalide that is also normally found in AMD.However, little is known about the impact of Fe(III)-binding ligand SCNˉ on schwertmannite stability and its subsequent capacity to bind trace elements. Here, we investigated the adsorption of SCNˉ on schwertmannite and subsequent mineral transformation to characterize this little-known process. The appearance of Fe2+indicated that the interactions between schwertmannite and SCNˉ may involve complexation and reduction reactions. Results showed that the majority of the adsorbed-SCNˉ was immobilized on schwertmannite during the 60-days transformation. The transformation rates of schwertmannite increased with increasing concentrations of SCNˉ. Goethite was detected as the dominant transformation product with or without SCNˉ. The mechanisms of SCNˉ-promoted dissolution of schwertmannite can be described as follows:(1) formation of Fe(III)–NCS complexes on the schwertmannite surface and in solution, a process which increases the reactivity of solid phase Fe(III);(2) the extraction of Fe(III) from schwertmannite by SCNˉ and subsequent schwertmannite dissolution; and(3) the formation of secondary minerals from extracted Fe(III). These findings may improve AMD treatment strategies and provide insight into the use and potential reuse of schwertmannite as a trace element sorbent.展开更多
Schwertmannite is an important Fe(Ⅲ)-oxyhydroxysulfate in acid mine drainage (AMD) polluted areas and its stability depends on surrounding environmental factors and previously bound elements.The treatment and neutral...Schwertmannite is an important Fe(Ⅲ)-oxyhydroxysulfate in acid mine drainage (AMD) polluted areas and its stability depends on surrounding environmental factors and previously bound elements.The treatment and neutralization of AMD normally involve the use of lime,which leads to the discharge of abundant Ca in the mining area.Such an environmental disturbance brings up an important and less considered problem of how the reductive transformation of schwertmannite associated with coexisting Ca occurred.Here,the Fe(Ⅱ)-mediated transformation of Ca-adsorbed schwertmannite and subsequent Ca repartitioning behaviors were investigated.Results showed that adsorbed Ca had a weak inhibitory effect on Fe(Ⅱ)-mediated schwertmannite transformation.Release of SO_(4)2-and SEM images both indicated that transformation rates of schwertmannite decreased under the influence of adsorbed Ca.XRD patterns indicated that adsorbed Ca altered schwertmannite transformation pathways and product compositions upon treatment with 0.4 mmol/L Fe(Ⅱ).The end products of Sch notably contained both goethite and lepidocrocite;however,transformation products of SchCa only contained goethite all along.Approximately 33.5%of the surface adsorbed-Ca was released into solution within 6 hr after Fe(Ⅱ) injection.Aqueous Ca behaved in a“first release and then im-mobilization”manner,which indicated dissolution and secondary mineralization drove Ca migration during the Fe(Ⅱ)-mediated transformation of SchCa.Adsorbed Ca blocked the surface sites for subsequent Fe(Ⅱ) adsorption,limited the Fe(Ⅱ)-Fe(Ⅲ) ETAE,and decreased the transformation rates.This work sheds light on the complex geochemical behavior of schwertmannite under the influences of environmental perturbations in AMD environments.展开更多
In this study, effects of water conditions （flooded, wet, or dry） and eggshell dosages （0, 0.1, 1.0, and 10.0 g/kg soil, respectively） on pH variation, content of unavailable state of heavy metals, form of heavy m...In this study, effects of water conditions （flooded, wet, or dry） and eggshell dosages （0, 0.1, 1.0, and 10.0 g/kg soil, respectively） on pH variation, content of unavailable state of heavy metals, form of heavy metals, and available nutritious element calcium （Ca） in acid soils contaminated with heavy metals were investigated, respectively. The soil samples were continuously cultivated indoors and analyzed by toxicity characteristic leaching procedure and community bureau of reference （BCR） sequential extraction procedure. The results showed that the addition of eggshell could effectively improve the pH of acid soil and increase it to neutral level. Moreover, the contents of unavailable state of heavy metals Cu, Zn, and Cd increased significantly. Furthermore, when the soil was cultivated under the flooded condition with 1.0 g/kg eggshell, the unavailable state ofCu, Zn, and Cd increased the most, and these heavy metals were transformed into residual state. On the other hand, the amount of available state of Ca increased to 432.19 from 73.34 mg/kg with the addition of 1.0 g/kg eggshell, which indicated that the addition of eggshell dramatically improved the available state of Ca. Therefore, eggshell could ameliorate the soil environment as it led to the decrease of available heavy metals and improvement of fertilization effectively. In a word, this study indicates that the addition of eggshell would be a new potential method for remediation of acid field soils contaminated with heavy metals.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.42077114 and 41771346)the Local Innovation and Entrepreneurship Team Project of Guangdong Special Support Program(No.2019BT02L218)Zhaoqing University Innovation Research Team Funding Project.
文摘Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing effluent and recycling of surfactant solutions.In this study,a molecular imprinting technique was applied to selectively sorb polybrominated diphenyl ethers(PBDEs)in soil washing effluent.The novel molecular imprinted polymers(MIPs)using different template molecules were synthesized by precipitation polymerization.Adsorption behaviors andmechanisms ofMIPs were studied through experiments and theoretical calculations.The results show that 4-bromo-4'-hydroxybiphenyl and toluene can be effective imprinting molecule for MIPs synthesis.The maximal adsorption capacity of selected dummy molecular imprinted polymer(D1-MIP)was 1032.36μmol/g,and that of part molecular imprinted polymer(P-MIP)was 981.13μmol/g.Their imprinting factors in 5 PBDEs adsorption ranged from 2.13 to 5.88,the recovery percentage of Triton X-100 can reach 99.09%,confirming the feasibility of reusing surfactant.Various PBDEs could be removed by MIPs,and Quantitative Structure Property Relationship analysis revealed that PBDEs’molecular volume,planarity,polarity,and hydrophobicity have major influences on their adsorption performance.DFT calculation revealed that Van derWaals force and hydrogen bonding played important roles during selective adsorption.These results can provide effective theoretical guidance for surfactant enhanced soil elution in practical engineering applications.
基金supported by the National Key Research and Development Program of China (No.2018YFC1802800)the National Natural Science Foundation of China (Nos.41673091, U1501234)+1 种基金Local Innovation and Entrepreneurship Team Project of Guangdong Special Support Program (No.2019BT02L218)the Guangdong Science and Technology Program ((No.2020B121201003)。
文摘Polycyclic aromatic hydrocarbons(PAHs), typical representatives of the persistent organic pollutants(POPs), have become ubiquitous in the environment.In this study, a novel microbial consortium QY1 that performed outstanding PAHs-degrading capacity has been enriched.The degradation characteristics of single and mixed PAHs treated with QY1 were studied, and the effect of biochar on biodegradation of mixed PAHs and the potential of biochar in PAHs-heavy metal combined pollution bioremediation were also investigated.Results showed that, in single substrate system, QY1 degraded 94.5% of 500 mg/L phenanthrene(PHE) and 17.8% of 10 mg/L pyrene(PYR) after 7 days, while in PHE-PYR mixture system, the biodegradation efficiencies of PHE(500 mg/L) and PYR(10 mg/L) reached 94.0%and 96.2%, respectively, since PHE served as co-metabolic substrate to have significantly improved PYR biodegradation.Notably, with the cooperation of biochar, the biodegradations of PHE and PYR were greatly accelerated.Further, biochar could reduce the adverse impact of heavy metals(Cd^(2+), Cu^(2+), Cr_(2)O_(7)^(2-)) on PYR biodegradation remarkably.The sequencing analysis revealed that Methylobacterium, Burkholderia and Stenotrophomonas were the dominant genera of QY1 in almost all treatments, indicating that these genera might play key roles in PAHs biodegradation.Overall, this study provided new insights into the efficient bioremediation of PAHs-contaminated site.
基金supported by the National Natural Science Foundation of China(Nos.U1501234,41673091,41573091)the National Key Research and Development Program of China(No.2018YFC1802800)
文摘The degradation of 2,2′,4,4′-tetrabromodiphenyl ether(BDE-47) by Pycnoporus sanguineus was investigated in order to explore the impact of the heavy metal Cu2+ on BDE-47 decomposition and the subsequent formation of metabolites, as well as to further elucidate the degradation mechanism of BDE-47. An increase in degradation rate from 18.63% to49.76% in the first four days and its stabilization at(51.26 ± 0.08)% in the following days of BDE-47 incubation were observed. The presence of Cu2+ at 1 and 2 mg/L was found to promote the degradation rate to 56.41% and 60.79%, respectively, whereas higher level of Cu2+(≥ 5 mg/L) inhibited the removal of BDE-47. The similar concentration effects of Cu2+ was also found on contents of fungal protein and amounts of metabolites. Both intracellular and extracellular enzymes played certain roles in BDE-47 transportation with the best degradation rate at 27.90% and 27.67% on the fourth and third day, individually. During the degradation of BDE-47, four types of hydroxylated polybrominated diphenyl ethers(OH-PBDEs), i.e., 6′-OH-BDE-47, 5′-OH-BDE-47, 4′-OH-BDE-17, 2′-OH-BDE-28, and two bromophenols, i.e., 2,4-DBP and 4-BP were detected and considered as degradation products. These metabolites were further removed by P. sanguineus at rates of 22.42%,23.01%, 27.04%, 27.96%, 64.21%, and 40.62%, respectively.
基金supported by the National Natural Science Foundation of China (Nos. 41330639 and 41720104004)the National Key Research and Development Program of China (No. 2017YFD0801000)
文摘Schwertmannite is an amorphous iron(III)-oxyhydroxysulfate that forms in acid mine drainage(AMD) environments. The characteristic of high heavy metal adsorption capability makes schwertmannite a potentially useful, environmentally friendly material in wastewater treatment. Unstable schwertmannite is prone to recrystallization.Understanding the mechanisms that induce schwertmannite labilization and affect its capacity to remove heavy metals are of great environmental and geochemical significance.Thiocyanate(SCNˉ) is a hazardous pseudohalide that is also normally found in AMD.However, little is known about the impact of Fe(III)-binding ligand SCNˉ on schwertmannite stability and its subsequent capacity to bind trace elements. Here, we investigated the adsorption of SCNˉ on schwertmannite and subsequent mineral transformation to characterize this little-known process. The appearance of Fe2+indicated that the interactions between schwertmannite and SCNˉ may involve complexation and reduction reactions. Results showed that the majority of the adsorbed-SCNˉ was immobilized on schwertmannite during the 60-days transformation. The transformation rates of schwertmannite increased with increasing concentrations of SCNˉ. Goethite was detected as the dominant transformation product with or without SCNˉ. The mechanisms of SCNˉ-promoted dissolution of schwertmannite can be described as follows:(1) formation of Fe(III)–NCS complexes on the schwertmannite surface and in solution, a process which increases the reactivity of solid phase Fe(III);(2) the extraction of Fe(III) from schwertmannite by SCNˉ and subsequent schwertmannite dissolution; and(3) the formation of secondary minerals from extracted Fe(III). These findings may improve AMD treatment strategies and provide insight into the use and potential reuse of schwertmannite as a trace element sorbent.
基金supported by the National Natural Science Foundation of China (Nos.42007363,41977277)Scientific Research Project of Chongqing Technology and Business University (No.KFJJ2019051)+3 种基金Science and Technology Research Projects of Chongqing Education Commission (No.KJQN202000814)Chongqing Science and Technology Commission of China (No.cstc2019jcyj-msxmX0647)Foundation for High-level Talents of Chongqing University of Arts and Sciences (No.R2018CH11)Innovation Group of New Technologies for Industrial Pollution Control of Chongqing Education Commission (No.CXQT19023)。
文摘Schwertmannite is an important Fe(Ⅲ)-oxyhydroxysulfate in acid mine drainage (AMD) polluted areas and its stability depends on surrounding environmental factors and previously bound elements.The treatment and neutralization of AMD normally involve the use of lime,which leads to the discharge of abundant Ca in the mining area.Such an environmental disturbance brings up an important and less considered problem of how the reductive transformation of schwertmannite associated with coexisting Ca occurred.Here,the Fe(Ⅱ)-mediated transformation of Ca-adsorbed schwertmannite and subsequent Ca repartitioning behaviors were investigated.Results showed that adsorbed Ca had a weak inhibitory effect on Fe(Ⅱ)-mediated schwertmannite transformation.Release of SO_(4)2-and SEM images both indicated that transformation rates of schwertmannite decreased under the influence of adsorbed Ca.XRD patterns indicated that adsorbed Ca altered schwertmannite transformation pathways and product compositions upon treatment with 0.4 mmol/L Fe(Ⅱ).The end products of Sch notably contained both goethite and lepidocrocite;however,transformation products of SchCa only contained goethite all along.Approximately 33.5%of the surface adsorbed-Ca was released into solution within 6 hr after Fe(Ⅱ) injection.Aqueous Ca behaved in a“first release and then im-mobilization”manner,which indicated dissolution and secondary mineralization drove Ca migration during the Fe(Ⅱ)-mediated transformation of SchCa.Adsorbed Ca blocked the surface sites for subsequent Fe(Ⅱ) adsorption,limited the Fe(Ⅱ)-Fe(Ⅲ) ETAE,and decreased the transformation rates.This work sheds light on the complex geochemical behavior of schwertmannite under the influences of environmental perturbations in AMD environments.
文摘In this study, effects of water conditions （flooded, wet, or dry） and eggshell dosages （0, 0.1, 1.0, and 10.0 g/kg soil, respectively） on pH variation, content of unavailable state of heavy metals, form of heavy metals, and available nutritious element calcium （Ca） in acid soils contaminated with heavy metals were investigated, respectively. The soil samples were continuously cultivated indoors and analyzed by toxicity characteristic leaching procedure and community bureau of reference （BCR） sequential extraction procedure. The results showed that the addition of eggshell could effectively improve the pH of acid soil and increase it to neutral level. Moreover, the contents of unavailable state of heavy metals Cu, Zn, and Cd increased significantly. Furthermore, when the soil was cultivated under the flooded condition with 1.0 g/kg eggshell, the unavailable state ofCu, Zn, and Cd increased the most, and these heavy metals were transformed into residual state. On the other hand, the amount of available state of Ca increased to 432.19 from 73.34 mg/kg with the addition of 1.0 g/kg eggshell, which indicated that the addition of eggshell dramatically improved the available state of Ca. Therefore, eggshell could ameliorate the soil environment as it led to the decrease of available heavy metals and improvement of fertilization effectively. In a word, this study indicates that the addition of eggshell would be a new potential method for remediation of acid field soils contaminated with heavy metals.
