We investigated the adsorption performance of five Fe-based MOFs(Fe-BTC,MIL-100(Fe),MIL-101(Fe),MIL-53(Fe)and MIL-88 C(Fe))for removal of antimonite(Sb(Ⅲ))and antimonate(Sb(Ⅴ))from water.Among these MOFs,MIL-101(Fe)...We investigated the adsorption performance of five Fe-based MOFs(Fe-BTC,MIL-100(Fe),MIL-101(Fe),MIL-53(Fe)and MIL-88 C(Fe))for removal of antimonite(Sb(Ⅲ))and antimonate(Sb(Ⅴ))from water.Among these MOFs,MIL-101(Fe)exhibited the best adsorption capacities for both Sb(Ⅲ)and Sb(Ⅴ)(151.8 and 472.8 mg/g,respectively)which were higher than those of most adsorbents previously reported.The effect of steric hindrance was evident during Sb removal using the Fe-based MOFs,and the proper diameter of the smallest cage windows/channels should be considered an important parameter during the evaluation and selection of MOFs.Additionally,the adsorption capacities of MIL-101(Fe)for Sb(Ⅴ)decreased with increasing initial p H values(from 3.0 to 8.0),while the opposite trend was observed for Sb(Ⅲ).Chloride,nitrate and sulfate ions had a negligible influence on Sb(Ⅴ)adsorption,while NO3-and SO42-improved Sb(Ⅲ)adsorption.This result implies that inner sphere complexes might form during both Sb(Ⅲ)and Sb(Ⅴ)adsorption.展开更多
Soils and waters are heavily contaminated by antimony in Xikuangshan(XKS)mine area.It is widely accepted that oxidative dissolution of sulfide minerals and aqueous dissolution are the most prevalent geochemical mechan...Soils and waters are heavily contaminated by antimony in Xikuangshan(XKS)mine area.It is widely accepted that oxidative dissolution of sulfide minerals and aqueous dissolution are the most prevalent geochemical mechanisms for the release of Sb to the environment.Bosea sp.AS-1 is an antimonite-oxidizer isolated from the mine slag in Xikuangshan Sb mine.Whole genome sequencing revealed the presence of multiple sulfur-oxidizing genes,antimony(Sb)metabolism genes and carbon fixation genes in AS-1 s genome.We therefore hypothesized that under oxic conditions,AS-1 could mediate the oxidation of sulfide and Sb(Ⅲ)in stibnite(Sb_(2)S_(3))and lead to the release of Sb.Indeed,strain AS-1 was discovered as an autotrophic Sb(Ⅲ)-oxidizer.Antimony mobilization studies conducted with strain AS-1showed significantly enhanced mobilization of Sb,and complete oxidation of released Sb and sulfur to Sb(V)and sulfate.In addition,AS-1 induced a faster release of Sb under heterotrophic condition,and new acicular minerals might form.These findings support the hypothesis that microorganisms play an important role in the mobilization and transformation of Sb in XKS mine area and may contribute to our further understanding of the Sb biogeochemical redox cycle in natural environment.展开更多
Ⅰ. INTRODUCTIONSodium Antimono Gallate (Code name Sb-273) is a sort of oral antimonial anti-Japanese schistosomiasis medicine. Through clinical appraisal, Sb-273 was officially accepted as of low toxicity, and since ...Ⅰ. INTRODUCTIONSodium Antimono Gallate (Code name Sb-273) is a sort of oral antimonial anti-Japanese schistosomiasis medicine. Through clinical appraisal, Sb-273 was officially accepted as of low toxicity, and since 1970, has been in production for general use for treatment of schistosomiasis. It is synthesized by the Institute of Medicine of Nanjing and is a powder of cream colour. By recrystallizing it in water solution, we obtained a colourless and transparent monocrystal bulk. Element composition form of展开更多
Microbial oxidation and the mechanism of Sb(Ⅲ)are key governing elements in biogeochemical cycling.A novel Sb oxidizing bacterium,Klebsiella aerogenes HC10,was attracted early and revealed that extracellular metaboli...Microbial oxidation and the mechanism of Sb(Ⅲ)are key governing elements in biogeochemical cycling.A novel Sb oxidizing bacterium,Klebsiella aerogenes HC10,was attracted early and revealed that extracellular metabolites were the main fractions driving Sb oxidation.However,linkages between the extracellular metabolite driven Sb oxidation process and mechanism remain elusive.Here,model phenolic and quinone compounds,i.e.,anthraquinone-2,6-disulfonate(AQDS)and hydroquinone(HYD),representing extracellular oxidants secreted by K.aerogenes HC10,were chosen to further study the Sb(Ⅲ)oxidation mechanism.N_(2)purging and free radical quenching showed that oxygen-induced oxidation accounted for 36.78%of Sb(Ⅲ)in the metabolite reaction system,while hydroxyl free radicals(·OH)accounted for 15.52%.·OH and H_(2)O_(2)are the main driving factors for Sb oxidation.Radical quenching,methanol purification and electron paramagnetic resonance(EPR)analysis revealed that·OH,superoxide radical(O_(2)^(•-))and semiquinone(SQ-•)were reactive intermediates of the phenolic induced oxidation process.Phenolic-induced ROS are one of the main oxidants in metabolites.Cyclic voltammetry(CV)showed that electron transfer of quinone also mediated Sb(Ⅲ)oxidation.Part of Sb(V)was scavenged by the formation of the secondary Sb(V)-bearing mineral mopungite[NaSb(OH)6]in the incubation system.Our study demonstrates the microbial role of oxidation detoxification and mineralization of Sb and provides scientific references for the biochemical remediation of Sb-contaminated soil.展开更多
基金supported by the National Natural Science Foundation of China (No. 41201302)the Natural Science Foundation of Shanghai (No. 17ZR1407000)the Fundamental Research Funds for the Central Universities (No. 222201514337)
文摘We investigated the adsorption performance of five Fe-based MOFs(Fe-BTC,MIL-100(Fe),MIL-101(Fe),MIL-53(Fe)and MIL-88 C(Fe))for removal of antimonite(Sb(Ⅲ))and antimonate(Sb(Ⅴ))from water.Among these MOFs,MIL-101(Fe)exhibited the best adsorption capacities for both Sb(Ⅲ)and Sb(Ⅴ)(151.8 and 472.8 mg/g,respectively)which were higher than those of most adsorbents previously reported.The effect of steric hindrance was evident during Sb removal using the Fe-based MOFs,and the proper diameter of the smallest cage windows/channels should be considered an important parameter during the evaluation and selection of MOFs.Additionally,the adsorption capacities of MIL-101(Fe)for Sb(Ⅴ)decreased with increasing initial p H values(from 3.0 to 8.0),while the opposite trend was observed for Sb(Ⅲ).Chloride,nitrate and sulfate ions had a negligible influence on Sb(Ⅴ)adsorption,while NO3-and SO42-improved Sb(Ⅲ)adsorption.This result implies that inner sphere complexes might form during both Sb(Ⅲ)and Sb(Ⅴ)adsorption.
基金supported by the National Natural Science Foundation of China(Nos.42077220 and 41877320)。
文摘Soils and waters are heavily contaminated by antimony in Xikuangshan(XKS)mine area.It is widely accepted that oxidative dissolution of sulfide minerals and aqueous dissolution are the most prevalent geochemical mechanisms for the release of Sb to the environment.Bosea sp.AS-1 is an antimonite-oxidizer isolated from the mine slag in Xikuangshan Sb mine.Whole genome sequencing revealed the presence of multiple sulfur-oxidizing genes,antimony(Sb)metabolism genes and carbon fixation genes in AS-1 s genome.We therefore hypothesized that under oxic conditions,AS-1 could mediate the oxidation of sulfide and Sb(Ⅲ)in stibnite(Sb_(2)S_(3))and lead to the release of Sb.Indeed,strain AS-1 was discovered as an autotrophic Sb(Ⅲ)-oxidizer.Antimony mobilization studies conducted with strain AS-1showed significantly enhanced mobilization of Sb,and complete oxidation of released Sb and sulfur to Sb(V)and sulfate.In addition,AS-1 induced a faster release of Sb under heterotrophic condition,and new acicular minerals might form.These findings support the hypothesis that microorganisms play an important role in the mobilization and transformation of Sb in XKS mine area and may contribute to our further understanding of the Sb biogeochemical redox cycle in natural environment.
文摘Ⅰ. INTRODUCTIONSodium Antimono Gallate (Code name Sb-273) is a sort of oral antimonial anti-Japanese schistosomiasis medicine. Through clinical appraisal, Sb-273 was officially accepted as of low toxicity, and since 1970, has been in production for general use for treatment of schistosomiasis. It is synthesized by the Institute of Medicine of Nanjing and is a powder of cream colour. By recrystallizing it in water solution, we obtained a colourless and transparent monocrystal bulk. Element composition form of
基金supported by the National Natural Science Foundation of China(No.42267001)the College Young and Middle-aged Teachers’Basic Ability Improvement Project of Guangxi,China(No.2023KY0393).
文摘Microbial oxidation and the mechanism of Sb(Ⅲ)are key governing elements in biogeochemical cycling.A novel Sb oxidizing bacterium,Klebsiella aerogenes HC10,was attracted early and revealed that extracellular metabolites were the main fractions driving Sb oxidation.However,linkages between the extracellular metabolite driven Sb oxidation process and mechanism remain elusive.Here,model phenolic and quinone compounds,i.e.,anthraquinone-2,6-disulfonate(AQDS)and hydroquinone(HYD),representing extracellular oxidants secreted by K.aerogenes HC10,were chosen to further study the Sb(Ⅲ)oxidation mechanism.N_(2)purging and free radical quenching showed that oxygen-induced oxidation accounted for 36.78%of Sb(Ⅲ)in the metabolite reaction system,while hydroxyl free radicals(·OH)accounted for 15.52%.·OH and H_(2)O_(2)are the main driving factors for Sb oxidation.Radical quenching,methanol purification and electron paramagnetic resonance(EPR)analysis revealed that·OH,superoxide radical(O_(2)^(•-))and semiquinone(SQ-•)were reactive intermediates of the phenolic induced oxidation process.Phenolic-induced ROS are one of the main oxidants in metabolites.Cyclic voltammetry(CV)showed that electron transfer of quinone also mediated Sb(Ⅲ)oxidation.Part of Sb(V)was scavenged by the formation of the secondary Sb(V)-bearing mineral mopungite[NaSb(OH)6]in the incubation system.Our study demonstrates the microbial role of oxidation detoxification and mineralization of Sb and provides scientific references for the biochemical remediation of Sb-contaminated soil.
