Arsenic(As)speciation transformation in acid mine drainage(AMD)is comprehensively affected by biological and abiotic factors,such as microbially mediated Fe/S redox reactions and changes in environmental conditions(pH...Arsenic(As)speciation transformation in acid mine drainage(AMD)is comprehensively affected by biological and abiotic factors,such as microbially mediated Fe/S redox reactions and changes in environmental conditions(pH and oxidation-reduction potential).However,their combined impacts on arsenic speciation transformation remain poorly studied.Therefore,we explored arsenic transformation and immobilization during pyrite dissolution mediated by AMD enrichment culture under different acidic pH conditions.The results for incubation and mineralogical transformation of solid residues show that in the presence of AMD enrichment culture,pH 2.0,2.5,and 3.0 are more conducive to the formation of jarosites and ferric arsenate,which could immobilize high quantities of dissolved arsenic by adsorption and coprecipitation.The pH conditions significantly affect the initial adsorption of microbial cells to the minerals and the evolution of microbial community structure,further infuencing the biodissolution of pyrite and the release and oxidation process of Fe/S.The results of Fe/S/As speciation transformation of the solid residues show that the transformation of Fe,S,and As in solution is mainly regulated by pH and potential values,which imposed significantly different effects on the formation of secondary minerals and thus arsenic oxidation and immobilization.The above results indicated that arsenic transformation is closely related to the Fe/S oxidation associated with pyrite bio-oxidation,and this correlation is critically regulated by the pH conditions of the system.展开更多
The role of Fe/S ratios(ω, g/g) in the uranium bioleaching from a complex uranium ore by Acidithiobacillus ferrooxidans and Acidithiobacillus thiooxidans consortium was investigated. The results showed good uranium e...The role of Fe/S ratios(ω, g/g) in the uranium bioleaching from a complex uranium ore by Acidithiobacillus ferrooxidans and Acidithiobacillus thiooxidans consortium was investigated. The results showed good uranium extraction with over 90% at the Fe/S ratio of 5:0.5, 5:1 and 5:5, while poor extraction(<46%) at the Fe/S ratio of 5:0 and 5:10.Furthermore, the bacterial community analysis based on species-specific gyrB numbers indicated that, absent sulfur or excessive sulfur would be not conducive to the synergistic growth for A. ferrooxidans and A. thiooxidans, and then not conducive to the uranium dissolution. Meanwhile, the sulfur-oxidizers could play an important role in the process of uranium synergistic bioleaching by mixed bacterial consortia. Additionally, the characteristics of mineral residue was detected by SEM-EDS. The results showed appropriate sulfur dosage would change the structure and improve the porosity of passivation substance. Lastly, the uranium dissolution kinetics and biochemical reaction mechanism was analyzed. It indicated that the biochemical reaction coupling iron and sulfur had a pleiotropic effect on the uranium dissolution from the ore particles, appropriate Fe/S ratio is the key factor for uranium bioleaching by chemoautotrophic acidophiles.展开更多
Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coup...Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by pyrolysis.The prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the reaction.Moreover,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation efficiency.Further,biochar can effectively promote cycling stability by limiting Fe leaching.This work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.展开更多
The migration and transformation of hexavalent chromium(Cr(VI))in the environment are regulated by pyrite(FeS2).However,variations in pyrite crystal facets influence the adsorption behavior and electron transfer betwe...The migration and transformation of hexavalent chromium(Cr(VI))in the environment are regulated by pyrite(FeS2).However,variations in pyrite crystal facets influence the adsorption behavior and electron transfer between pyrite and Cr(VI),thereby impacting the Cr(VI)reduction performance.Herein,two naturally common facets of pyritewere synthesized hydrothermally to investigate the facet-dependent mechanisms of Cr(VI)reduction.The experimental results revealed that the{111}facet exhibited approximately 1.30–1.50 times higher efficiency in Cr(VI)reduction compared to the{100}facet.Surface analyses and electrochemical results indicated that{111}facet displayed a higher iron-sulfur oxidation level,which was affected by its superior electrochemical properties during the reaction with Cr(VI).Density functional theory(DFT)calculations demonstrated that the narrower band gap and lower work function on{111}facet were more favorable for the electron transfer between Fe(II)and Cr(VI).Furthermore,different adsorption configurations were observed on{100}and{111}surfaces due to the unique arrangements of Fe and S atoms.Specifically,O atoms in Cr_(2)O_(7)^(2−)directly bound with the S sites on{100}but the Fe sites on{111}.According to the density of states(DOS),the Fe site had better reactivity than the S site in the reaction,which appeared to be related to the fracture of S-S bonds.Additionally,the adsorption configuration of Cr_(2)O_(7)^(2−)on{111}surface showed a stronger adsorption energy and a more stable coordination mode,favoring subsequent Cr(VI)reduction process.These findings provide an in-depth analysis of facet-dependent mechanisms underlying Cr(VI)reduction behavior,offering new insights into studying environmental interactions between heavy metals and natural minerals.展开更多
基金supported by the National Natural Science Foundation of China (NSFC) (No.41830318)the Joint Funds of the NSFC-DFG (No.51861135305)。
文摘Arsenic(As)speciation transformation in acid mine drainage(AMD)is comprehensively affected by biological and abiotic factors,such as microbially mediated Fe/S redox reactions and changes in environmental conditions(pH and oxidation-reduction potential).However,their combined impacts on arsenic speciation transformation remain poorly studied.Therefore,we explored arsenic transformation and immobilization during pyrite dissolution mediated by AMD enrichment culture under different acidic pH conditions.The results for incubation and mineralogical transformation of solid residues show that in the presence of AMD enrichment culture,pH 2.0,2.5,and 3.0 are more conducive to the formation of jarosites and ferric arsenate,which could immobilize high quantities of dissolved arsenic by adsorption and coprecipitation.The pH conditions significantly affect the initial adsorption of microbial cells to the minerals and the evolution of microbial community structure,further infuencing the biodissolution of pyrite and the release and oxidation process of Fe/S.The results of Fe/S/As speciation transformation of the solid residues show that the transformation of Fe,S,and As in solution is mainly regulated by pH and potential values,which imposed significantly different effects on the formation of secondary minerals and thus arsenic oxidation and immobilization.The above results indicated that arsenic transformation is closely related to the Fe/S oxidation associated with pyrite bio-oxidation,and this correlation is critically regulated by the pH conditions of the system.
基金Project(51804165) supported by the National Natural Science Foundation of ChinaProject(2018JJ3441) supported by the Natural Science Foundation of Hunan Province,China。
文摘The role of Fe/S ratios(ω, g/g) in the uranium bioleaching from a complex uranium ore by Acidithiobacillus ferrooxidans and Acidithiobacillus thiooxidans consortium was investigated. The results showed good uranium extraction with over 90% at the Fe/S ratio of 5:0.5, 5:1 and 5:5, while poor extraction(<46%) at the Fe/S ratio of 5:0 and 5:10.Furthermore, the bacterial community analysis based on species-specific gyrB numbers indicated that, absent sulfur or excessive sulfur would be not conducive to the synergistic growth for A. ferrooxidans and A. thiooxidans, and then not conducive to the uranium dissolution. Meanwhile, the sulfur-oxidizers could play an important role in the process of uranium synergistic bioleaching by mixed bacterial consortia. Additionally, the characteristics of mineral residue was detected by SEM-EDS. The results showed appropriate sulfur dosage would change the structure and improve the porosity of passivation substance. Lastly, the uranium dissolution kinetics and biochemical reaction mechanism was analyzed. It indicated that the biochemical reaction coupling iron and sulfur had a pleiotropic effect on the uranium dissolution from the ore particles, appropriate Fe/S ratio is the key factor for uranium bioleaching by chemoautotrophic acidophiles.
基金financially supported by the National Natural Science Foundation of China (Nos.21876139 and 21922606)Yulin Science and Technology Project of China (No.CXY2021-134)。
文摘Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater treatment.Here,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by pyrolysis.The prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the reaction.Moreover,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation efficiency.Further,biochar can effectively promote cycling stability by limiting Fe leaching.This work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.
基金supported by the National Natural Science Foundation of China(No.42277256)the Natural Science Foundation of Hunan Province(No.2022JJ30710)+1 种基金Hunan Province Environmental Protection Research Program(No.HBKT-2021014)Guangdong Province Dabaoshan Mining Co.Ltd Technology Program(Semi-industrial test of 200T/time low-grade copper ore bio-heap leaching).
文摘The migration and transformation of hexavalent chromium(Cr(VI))in the environment are regulated by pyrite(FeS2).However,variations in pyrite crystal facets influence the adsorption behavior and electron transfer between pyrite and Cr(VI),thereby impacting the Cr(VI)reduction performance.Herein,two naturally common facets of pyritewere synthesized hydrothermally to investigate the facet-dependent mechanisms of Cr(VI)reduction.The experimental results revealed that the{111}facet exhibited approximately 1.30–1.50 times higher efficiency in Cr(VI)reduction compared to the{100}facet.Surface analyses and electrochemical results indicated that{111}facet displayed a higher iron-sulfur oxidation level,which was affected by its superior electrochemical properties during the reaction with Cr(VI).Density functional theory(DFT)calculations demonstrated that the narrower band gap and lower work function on{111}facet were more favorable for the electron transfer between Fe(II)and Cr(VI).Furthermore,different adsorption configurations were observed on{100}and{111}surfaces due to the unique arrangements of Fe and S atoms.Specifically,O atoms in Cr_(2)O_(7)^(2−)directly bound with the S sites on{100}but the Fe sites on{111}.According to the density of states(DOS),the Fe site had better reactivity than the S site in the reaction,which appeared to be related to the fracture of S-S bonds.Additionally,the adsorption configuration of Cr_(2)O_(7)^(2−)on{111}surface showed a stronger adsorption energy and a more stable coordination mode,favoring subsequent Cr(VI)reduction process.These findings provide an in-depth analysis of facet-dependent mechanisms underlying Cr(VI)reduction behavior,offering new insights into studying environmental interactions between heavy metals and natural minerals.
