The rapid development of nanoscience and nanotechnology, with thousands types of nanomaterials being produced, will lead to various environmental impacts. Thus,understanding the behaviors and fate of these nanomateria...The rapid development of nanoscience and nanotechnology, with thousands types of nanomaterials being produced, will lead to various environmental impacts. Thus,understanding the behaviors and fate of these nanomaterials is essential. This study focused on the interaction between polyhydroxy fullerenes（PHF） and ferrihydrite（Fh）, a widespread iron（oxyhydr）oxide nanomineral and geosorbent. Our results showed that PHF were effectively adsorbed by Fh. The adsorption isotherm fitted the D-R model well, with an adsorption capacity of 67.1 mg/g. The adsorption mean free energy of 10.72 k J/mol suggested that PHF were chemisorbed on Fh. An increase in the solution p H and a decrease of the Fh surface zeta potential were observed after the adsorption of PHF on Fh; moreover, increasing initial solution p H led to a reduction of adsorption. The Fourier transform infrared spectra detected a red shift of C–O stretching from 1075 to 1062 cm-1 and a decrease of Fe–O bending, implying the interaction between PHF oxygenic functional groups and Fh surface hydroxyls. On the other hand, PHF affected the aggregation and reactivity of Fh by changing its surface physicochemical properties. Aggregation of PHF and Fh with individual particle sizes increasing from 2 nm to larger than 5 nm was measured by atomic force microscopy. The uniform distribution of C and Fe suggested that the aggregates of Fh were possibly bridged by PHF. Our results indicated that the interaction between PHF and Fh could evidently influence the migration of PHF, as well as the aggregation and reactivity of Fh.展开更多
Microbially mediated bioreduction of iron oxyhydroxide plays an important role in the biogeochemical cycle of iron.Geobacter sulfurreducens is a representative dissimilatory ironreducing bacterium that assembles elect...Microbially mediated bioreduction of iron oxyhydroxide plays an important role in the biogeochemical cycle of iron.Geobacter sulfurreducens is a representative dissimilatory ironreducing bacterium that assembles electrically conductive pili and cytochromes.The impact of supplementation withγ-Fe_2O_3 nanoparticles(NPs)(0.2 and 0.6 g)on the G.sulfurreducens-mediated reduction of ferrihydrite was investigated.In the overall performance of microbial ferrihydrite reduction mediated byγ-Fe_2O_3 NPs,stronger reduction was observed in the presence of direct contact withγ-Fe_2O_3 NPs than with indirect contact.Compared to the production of Fe(Ⅱ)derived from biotic modification with ferrihydrite alone,increases greater than 1.6-and 1.4-fold in the production of Fe(Ⅱ)were detected in the biotic modifications in which direct contact with 0.2 g and 0.6 gγ-Fe_2O_3 NPs,respectively,occurred.X-ray diffraction analysis indicated that magnetite was a unique representative iron mineral in ferrihydrite when active G.sulfurreducens cells were in direct contact withγ-Fe_2O_3 NPs.Because of the sorption of biogenic Fe(Ⅱ)ontoγ-Fe_2O_3 NPs instead of ferrihydrite,the addition ofγ-Fe_2O_3 NPs could also contribute to increased duration of ferrihydrite reduction by preventing ferrihydrite surface passivation.Additionally,electron microscopy analysis confirmed that the direct addition ofγ-Fe_2O_3 NPs stimulated the electrically conductive pili and cytochromes to stretch,facilitating long-range electron transfer between the cells and ferrihydrite.The obtained findings provide a more comprehensive understanding of the effects of iron oxide NPs on soil biogeochemistry.展开更多
Fe5O7(OH)4H2O ferrihydrite is a low-crystallinity antiferromagnetic material.c-Fe2O3(maghemite)magnetic nanoparticles were prepared from a ferrihydrite precursor,by chemically induced transformation in FeCl2/NaOH solu...Fe5O7(OH)4H2O ferrihydrite is a low-crystallinity antiferromagnetic material.c-Fe2O3(maghemite)magnetic nanoparticles were prepared from a ferrihydrite precursor,by chemically induced transformation in FeCl2/NaOH solution.The magnetization,morphology,crystal structure and chemical composition of the products were determined by vibrating sample magnetometry,transmission electron microscopy,X-ray diffraction(XRD),energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy(XPS).Ferrihydrite underwent aggregation growth and transformed into a-FeO(OH)(goethite)particles,which subsequently transformed into c-Fe2O3nanoparticles,that became coated with NaCl.The c-Fe2O3particles had a flake-like morphology,when prepared from 0.01 mol/L FeCl2and a FeCl2:NaOH molar ratio of 0.4.The c-Fe2O3particles were more spherical,when prepared from a FeCl2:NaOH molar ratio of 0.6.The Fe content of the flake-like particles was lower than that of the spherical particles.Their magnetizations were similar,and the coercivity of the flake-like particles was larger.The differences in morphology and magnetization were attributed to the surface effect,and the difference in coercivity to the shape effect.展开更多
基金supported by the National Natural Science Foundation of China(No.41572031)the National Program for Support of Top-notch Young Professionals,Guangdong Provincial Youth Top-notch Talent Support Program(No.2014TQ01Z249)+1 种基金the Newton Advanced Fellowship Through the Royal Society in the United Kingdom(No.NA150190)the National Key Research and Development Plan(No.2016YFD0800700)
文摘The rapid development of nanoscience and nanotechnology, with thousands types of nanomaterials being produced, will lead to various environmental impacts. Thus,understanding the behaviors and fate of these nanomaterials is essential. This study focused on the interaction between polyhydroxy fullerenes（PHF） and ferrihydrite（Fh）, a widespread iron（oxyhydr）oxide nanomineral and geosorbent. Our results showed that PHF were effectively adsorbed by Fh. The adsorption isotherm fitted the D-R model well, with an adsorption capacity of 67.1 mg/g. The adsorption mean free energy of 10.72 k J/mol suggested that PHF were chemisorbed on Fh. An increase in the solution p H and a decrease of the Fh surface zeta potential were observed after the adsorption of PHF on Fh; moreover, increasing initial solution p H led to a reduction of adsorption. The Fourier transform infrared spectra detected a red shift of C–O stretching from 1075 to 1062 cm-1 and a decrease of Fe–O bending, implying the interaction between PHF oxygenic functional groups and Fh surface hydroxyls. On the other hand, PHF affected the aggregation and reactivity of Fh by changing its surface physicochemical properties. Aggregation of PHF and Fh with individual particle sizes increasing from 2 nm to larger than 5 nm was measured by atomic force microscopy. The uniform distribution of C and Fe suggested that the aggregates of Fh were possibly bridged by PHF. Our results indicated that the interaction between PHF and Fh could evidently influence the migration of PHF, as well as the aggregation and reactivity of Fh.
基金supported by the National Natural Science Foundation of China (Nos. 41571449, 41271260, 41276101 and 41807035)the Fundamental Research Fund for the Central Universities of China (No. 20720160083)+2 种基金the Natural Science Foundation of Fujian Province of China (Nos. 2018J05073 and 2018Y0074)the Project of Educational Scientific Research of Fujian Province of China (Nos. JAT170831 and JA13344)the Open Fund of Key Laboratory of Measurement and Control System for Coastal Environment of China (No. S1-KF1701)
文摘Microbially mediated bioreduction of iron oxyhydroxide plays an important role in the biogeochemical cycle of iron.Geobacter sulfurreducens is a representative dissimilatory ironreducing bacterium that assembles electrically conductive pili and cytochromes.The impact of supplementation withγ-Fe_2O_3 nanoparticles(NPs)(0.2 and 0.6 g)on the G.sulfurreducens-mediated reduction of ferrihydrite was investigated.In the overall performance of microbial ferrihydrite reduction mediated byγ-Fe_2O_3 NPs,stronger reduction was observed in the presence of direct contact withγ-Fe_2O_3 NPs than with indirect contact.Compared to the production of Fe(Ⅱ)derived from biotic modification with ferrihydrite alone,increases greater than 1.6-and 1.4-fold in the production of Fe(Ⅱ)were detected in the biotic modifications in which direct contact with 0.2 g and 0.6 gγ-Fe_2O_3 NPs,respectively,occurred.X-ray diffraction analysis indicated that magnetite was a unique representative iron mineral in ferrihydrite when active G.sulfurreducens cells were in direct contact withγ-Fe_2O_3 NPs.Because of the sorption of biogenic Fe(Ⅱ)ontoγ-Fe_2O_3 NPs instead of ferrihydrite,the addition ofγ-Fe_2O_3 NPs could also contribute to increased duration of ferrihydrite reduction by preventing ferrihydrite surface passivation.Additionally,electron microscopy analysis confirmed that the direct addition ofγ-Fe_2O_3 NPs stimulated the electrically conductive pili and cytochromes to stretch,facilitating long-range electron transfer between the cells and ferrihydrite.The obtained findings provide a more comprehensive understanding of the effects of iron oxide NPs on soil biogeochemistry.
基金supported by the National Natural Science Foundation of China (51375039 and 11074205)
文摘Fe5O7(OH)4H2O ferrihydrite is a low-crystallinity antiferromagnetic material.c-Fe2O3(maghemite)magnetic nanoparticles were prepared from a ferrihydrite precursor,by chemically induced transformation in FeCl2/NaOH solution.The magnetization,morphology,crystal structure and chemical composition of the products were determined by vibrating sample magnetometry,transmission electron microscopy,X-ray diffraction(XRD),energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy(XPS).Ferrihydrite underwent aggregation growth and transformed into a-FeO(OH)(goethite)particles,which subsequently transformed into c-Fe2O3nanoparticles,that became coated with NaCl.The c-Fe2O3particles had a flake-like morphology,when prepared from 0.01 mol/L FeCl2and a FeCl2:NaOH molar ratio of 0.4.The c-Fe2O3particles were more spherical,when prepared from a FeCl2:NaOH molar ratio of 0.6.The Fe content of the flake-like particles was lower than that of the spherical particles.Their magnetizations were similar,and the coercivity of the flake-like particles was larger.The differences in morphology and magnetization were attributed to the surface effect,and the difference in coercivity to the shape effect.
