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1.
Jinlong Yan Tao Jiang Ying Yao Jun Wang Yuanli Cai Nelson W. Green Shiqiang Wei 《环境科学学报(英文版)》2017,29(5):197-205
The phosphorus(P) fraction distribution and formation mechanism in the supernatant after P adsorption onto iron oxides and iron oxide-humic acid(HA) complexes were analyzed using the ultrafiltration method in this study.With an initial P concentration of 20 mg/L(I =0.01 mol/L and pH = 7),it was shown that the colloid(1 kDa-0.45 μm) component of P accounted for 10.6%,11.6%,6.5%,and 4.0%of remaining total P concentration in the supernatant after P adsorption onto ferrihydrite(FH),goethite(GE),ferrihydrite-humic acid complex(FH-HA),goethite-humic acid complex(GE-HA),respectively.The 1 kDa component of P was still the predominant fraction in the supernatant,and underestimated colloidal P accounted for 2.2%,55.1%,45.5%,and 38.7%of P adsorption onto the solid surface of FH,FH-HA,GE and GE-HA,respectively.Thus,the colloid P could not be neglected.Notably,it could be interpreted that Fe~(3+) hydrolysis from the adsorbents followed by the formation of colloidal hydrous ferric oxide aggregates was the main mechanism for the formation of the colloid P in the supernatant.And colloidal adsorbent particles co-existing in the supernatant were another important reason for it.Additionally,dissolve organic matter dissolved from iron oxide-HA complexes could occupy large adsorption sites of colloidal iron causing less colloid P in the supernatant.Ultimately,we believe that the findings can provide a new way to deeply interpret the geochemical cycling of P,even when considering other contaminants such as organic pollutants,heavy metal ions,and arsenate at the sediment/soil-water interface in the real environment. 相似文献
2.
《环境科学学报(英文版)》2020,(2)
Fe–Mn binary oxide(FMBO) possesses high efficiency for As(Ⅲ) abatement based on the good adsorption affinity of iron oxide and the oxidizing capacity of Mn(Ⅳ), and the composition and structure of FMBO play important roles in this process.To compare the removal performance and determine the optimum formula for FMBO, magnetic graphene oxide(MRGO)–FMBO and MRGO–MnO_2 were synthesized with MRGO as a carrier to improve the dispersity of the adsorbents in aquifers and achieve magnetic recycling.Results indicated that MRGO–FMBO had higher As(Ⅲ) removal than that of MRGO–MnO_2,although the ratios of Fe and Mn were similar, because the binary oxide of Fe and Mn facilitated electron transfer from Mn(Ⅳ) to As(Ⅲ), while the separation of Mn and Fe on MRGO–MnO_2 restricted the process.The optimal stoichiometry x for MRGO–FMBO(Mn_xFe_(3-x)O_4) was 0.46, and an extraordinary adsorption capacity of 24.38 mg/g for As(Ⅲ) was achieved.MRGO–FMBO showed stable dispersive properties in aquifers, and exhibited excellent practicability and reusability, with a saturation magnetization of 7.6 emu/g and high conservation of magnetic properties after 5 cycles of regeneration and reuse.In addition, the presence of coexisting ions would not restrict the practical application of MRGO–FMBO in groundwater remediation.The redox reactions of As(Ⅲ) and Mn(Ⅳ) on MRGO–FMBO were also described.The deprotonated aqueous As(Ⅲ) on the surface of MRGO–FMBO transferred electrons to Mn(Ⅳ), and the formed As(Ⅴ) oxyanions were bound to ferric oxide as inner-sphere complexes by coordinating their "–OH" groups with Mn(Ⅳ)oxides at the surface of MRGO–FMBO.This work could provide new insights into highperformance removal of As(Ⅲ) in aquifers. 相似文献
3.
Fe–Mn binary oxide (FMBO) possesses high efficiency for As(III) abatement based on the good adsorption affinity of iron oxide and the oxidizing capacity of Mn(IV), and the composition and structure of FMBO play important roles in this process. To compare the removal performance and determine the optimum formula for FMBO, magnetic graphene oxide (MRGO)–FMBO and MRGO–MnO2 were synthesized with MRGO as a carrier to improve the dispersity of the adsorbents in aquifers and achieve magnetic recycling. Results indicated that MRGO–FMBO had higher As(III) removal than that of MRGO–MnO2, although the ratios of Fe and Mn were similar, because the binary oxide of Fe and Mn facilitated electron transfer from Mn(IV) to As(III), while the separation of Mn and Fe on MRGO–MnO2 restricted the process. The optimal stoichiometry x for MRGO–FMBO (MnxFe3-xO4) was 0.46, and an extraordinary adsorption capacity of 24.38 mg/g for As(III) was achieved. MRGO–FMBO showed stable dispersive properties in aquifers, and exhibited excellent practicability and reusability, with a saturation magnetization of 7.6 emu/g and high conservation of magnetic properties after 5 cycles of regeneration and reuse. In addition, the presence of coexisting ions would not restrict the practical application of MRGO–FMBO in groundwater remediation. The redox reactions of As(III) and Mn(IV) on MRGO–FMBO were also described. The deprotonated aqueous As(III) on the surface of MRGO–FMBO transferred electrons to Mn(IV), and the formed As(V) oxyanions were bound to ferric oxide as inner-sphere complexes by coordinating their “–OH” groups with Mn(IV) oxides at the surface of MRGO–FMBO. This work could provide new insights into high-performance removal of As(III) in aquifers. 相似文献
4.
Zhonglan Yang Lingyu Bai Shiming Su Yanan Wang Cuixia Wu Xibai Zeng Benhua Sun 《环境科学学报(英文版)》2021,33(2):43-50
During the aging process, ferrihydrite was transformed into mineral mixtures composed of different proportions of ferrihydrite, goethite, lepidocrocite and hematite. Such a transformation may affect the fixed ability of arsenic. In this study, the stability of Fe-As composites formed with As(V) and the minerals aged for 0, 1, 4, 10 and 30 days of ferrihydrite were systematically examined, and the effects of molar of ratios Fe/As were also clarified using kinetic methods combined with multiple spectroscopic techniques. The results indicated that As(V) was rapidly adsorbed on minerals during the initial polymerization process, which delayed both the ferrihydrite conversion and the hematite formation. When the Fe/As molar ratio was 1.875 and 5.66, the As(V) adsorbed by ferrihydrite began to release after 6 hr and 12 hr, respectively. The corresponding release amounts of As(V) were 0.55 g/L and 0.07 g/L, and the adsorption rates were 92.43% and 97.50% at 60 days, respectively. However, the As(V) adsorbed by the transformation products aged for 30 days of ferrihydrite began to release after adsorbed 30 days. The corresponding release amounts of As(V) were 0.25 g/L and 0.03 g/L, and the adsorption rates were 84.23% and 92.18% after adsorbed 60 days, for the Fe/As=1.875 and 5.66, respectively. Overall, the combination of As(V) with ferrihydrite and aged products transformed from a thermodynamically metastable phase to a dynamically stable state within a certain duration. Moreover, the aging process of ferrihydrite reduced the sorption ability of arsenate by iron (hydr)oxide but enhanced the stability of the Fe-As composites. 相似文献
5.
Santosh Kumar Mohmmad Y. Wani Joonseok Koh João M. Gil Abilio J.F.N. Sobral 《环境科学学报(英文版)》2018,30(7):77-84
One of today's major challenges is to provide green materials for a cleaner environment. We have conducted studies on carbon dioxide(CO2) adsorption and conversion to valuable products by an ecofriendly approach based in chitosan/graphene oxide(CSGO) nanocomposite film. Rheological behavior indicates that the CSGO has a better solvation property than the pure chitosan. An adsorption capacity of 1.0152 mmol CO_2/g of CSGO nanocomposite at4.6 bar was observed. The catalytic behavior of the CSGO nanocomposite in the presence of tetra-n-butylammonium iodide(n-Bu4 NI) as co-catalyst was evaluated for the cycloaddition of CO_2 to epoxides, to give cyclic carbonates, in the absence of any solvent. These results strongly suggest that the CSGO nanocomposite may open new vistas towards the development of ecofriendly material for catalytic conversion and adsorption of CO_2 on industrial scale. 相似文献
6.
Mg–Al–Fe layered double hydroxides(LDHs) were exfoliated and incorporated in polyether sulfone membranes for the removal of phosphate and fluoride for the first time. The exfoliation methods, coagulation bath, LDH amount, interfering ions, adsorption isotherm,desorption and reuse of the membranes were investigated. It was found that LDHs could be quickly exfoliated in formamide/N,N-dimethylformamide(DMF) solvent mixtures with sodium carboxymethyl cellulose as a stabilizer. The membranes displayed much higher adsorption capacity for phosphate(5.61 mg/g) and faster adsorption rate than the unexfoliated materials. With increased DMF content in the coagulation bath, the static and dynamic adsorption capacity rose. Interference from Cl-and SO_4~(2-)(50 mg/L) on adsorption of phosphates was not apparent. The membranes displayed excellent reusability in dynamic adsorption/desorption. The membranes also showed high adsorption capacity for fluorides(1.61 mg/g). 相似文献
7.
To obtain a cost-effective adsorbent for the removal of arsenic in water,a novel nanostructured Fe–Co based metal organic framework(MOF-74)adsorbent was successfully prepared via a simple solvothermal method.The adsorption experiments showed that the optimal molar ratio of Fe/Co in the adsorbent was 2:1.The Fe_2Co_1MOF-74 was characterized by various techniques and the results showed that the nanoparticle diameter ranged from60 to 80 nm and the specific surface area was 147.82 m~2/g.The isotherm and kinetic parameters of arsenic removal on Fe_2Co_1MOF-74 were well-fitted by the Langmuir and pseudo-second-order models.The maximum adsorption capacities toward As(III)and As(V)were 266.52 and 292.29 mg/g,respectively.The presence of sulfate,carbonate and humic acid had no obvious effect on arsenic adsorption.However,coexisting phosphate significantly hindered the removal of arsenic,especially at high concentrations(10 mmol/L).Electrostatic interaction and hydroxyl and metal–oxygen groups played important roles in the adsorption of arsenic.Furthermore,the prepared adsorbent had stable adsorption ability after regeneration and when used in a real-water matrix.The excellent adsorption performance of Fe_2Co_1MOF-74 material makes it a potentially promising adsorbent for the removal of arsenic. 相似文献
8.
In this study, greatly enhanced Mn(II) adsorption was achieved by as-synthesized diethylenetriaminepentaacetate acid intercalated Mg/Al layered double hydroxides(LDHsDTPA). The adsorption capacity of LDHs-DTPA was 83.5 mg/g, which is much higher than that of LDHs-EDTA(44.4 mg/g), LDHs-Oxalate(21.6 mg/g) and LDHs(28.8 mg/g). The adsorption data of aqueous Mn(II) using LDHs-DTPA could be well described by the pseudosecond order kinetics and Langmuir isotherm model. Thermodynamics study results also showed that the adsorption process of Mn(II) by LDHs-DTPA was exothermic as indicated by the negative ΔH value. Furthermore, based on the structural, morphological and thermostable features, as well as FT-IR and XPS characterizations of LDHs-DTPA and the pristine LDHs, the adsorption mechanism of Mn(II) was proposed. The carboxyl groups of DTPA were proposed to be the main binding sites for Mn(II), and the hydroxyl groups of LDHs also played a minor role in the adsorption process. Among the three common regeneration reagents, 0.1 mol/L Na_2CO_3 was the best for reusing LDHs-DTPA in Mn(II)adsorption. Besides, the Mn(II) adsorption performance could be hindered in the presence of typical inorganic ions, especially cations. Further specific modifications of LDHs-DTPA are suggested to get more selective adsorption of Mn(II) in practical applications. 相似文献
9.
In order to study the influences of functionalized groups onto the adsorption of tetracycline (TC), we prepared a series of amino and amino–Fe3 + complex mesoporous silica adsorbents with diverse content of amino and Fe3 + groups (named N,N-SBA15 and Fe-N,N-SBA15). The resulting mesoporous silica adsorbents were fully characterized by X-ray powder diffraction, Fourier transform infrared spectrometer and N2 adsorption/desorption isotherms. Furthermore, the effects of functionalized groups on the removal of TC were investigated. The results showed that the periodic ordered structure of SBA-15 was maintained after modification of amino/Fe3 + groups. The functionalized amino groups decreased the adsorption capacity while the coordinated Fe3 + increased the adsorption capacity. The adsorption kinetics of TC fitted pseudo-second-order model well and the equilibrium was achieved quickly. The adsorption isotherms fitted the Langmuir model well and with the Fe3 + content increased from 3.93% to 8.26%, the Qmax of the adsorbents increased from 102 to 188 mmol/kg. The solution pH affected the adsorption of TC onto amino complex adsorbents slightly while influenced the adsorption onto Fe-amine complex adsorbents greatly. The adsorption of TC on SBA15 and N,N-SBA15 may be related to the formation of outer-sphere surface complexes, while the adsorption of TC onto Fe-N,N-SBA15 was mainly attributed to the inner-sphere surface complexes. This study could offer potential materials that have excellent adsorption behavior for environmental remediation and suggested useful information for the preparing other adsorbents in environmental applications. 相似文献
10.
Removal of Pb~(2+)and biodegradation of organophosphorus have been both widely investigated respectively. However, bio-remediation of both Pb~(2+)and organophosphorus still remains largely unexplored. Bacillus subtilis FZUL-33, which was isolated from the sediment of a lake, possesses the capability for both biomineralization of Pb~(2+)and biodegradation of acephate. In the present study, both Pb~(2+)and acephate were simultaneously removed via biodegradation and biomineralization in aqueous solutions.Batch experiments were conducted to study the influence of p H, interaction time and Pb~(2+)concentration on the process of removal of Pb2+. At the temperature of 25°C, the maximum removal of Pb~(2+)by B. subtilis FZUL-33 was 381.31 ± 11.46 mg/g under the conditions of p H 5.5, initial Pb~(2+)concentration of 1300 mg/L, and contact time of 10 min. Batch experiments were conducted to study the influence of acephate on removal of Pb~(2+)and the influence of Pb2+on biodegradation of acephate by B. subtilis FZUL-33. In the mixed system of acephate–Pb2+, the results show that biodegradation of acephate by B. subtilis FZUL-33 released PO43+, which promotes mineralization of Pb2+. The process of biodegradation of acephate was affected slightly when the concentration of Pb2+was below 100 mg/L. Based on the results, it can be inferred that the B. subtilis FZUL-33 plays a significant role in bio-remediation of organophosphorus-heavy metal compound contamination. 相似文献
11.
The characteristics of Pb2+ adsorption on the surface of birnessites with different average oxidation states (AOS) of Mn, synthesized under acidic and alkali conditions, were investigated. The results indicated that the amount of adsorbed Pb2+ increased with the increase of Mn AOS in birnessites. The amount of Pb2+ adsorbed positively correlated with the amount of released Mn2+, H+, and K+ (r = 0.9962 > 0.6614, n = 14, α = 0.01). The released Mn2+, H+, and K+ were derived mostly from the corresponding catio... 相似文献
12.
Ni/Fe-Fe_3O_4 nanocomposites were synthesized for dechlorination of 2,4-dichlorophenol(2,4-DCP). The effects of the Ni content in Ni/Fe-Fe_3O_4 nanocomposites, solution pH, and common dissolved ions on the dechlorination efficiency were investigated, in addition to the reusability of the nanocomposites. The results showed that increasing content of Ni in Ni/Fe–Fe_3O_4 nanocomposites, from 1 to 5 wt.%, greatly increased the dechlorination efficiency; the Ni/Fe–Fe_3O_4 nanocomposites had much higher dechlorination efficiency than bare Ni/Fe nanoparticles. Ni content of 5 wt.% and initial p H below 6.0 was found to be the optimal conditions for the catalytic dechlorination of 2,4-DCP. Both 2,4-DCP and the intermediate product 2-chlorophenol(2-CP) were completely removed, and the concentration of the final product phenol was close to the theoretical phenol production from complete dechlorination of 20 mg/L of 2,4-DCP, after 3 hr reaction at initial p H value of 6.0,3 g/L Ni/Fe-Fe_3O_4 , 5 wt.% Ni content in the composite, and temperature of 22℃. 2,4-DCP dechlorination was enhanced by Cl-and inhibited by NO3-and SO_4~(2-). The nanocomposites were easily separated from the solution by an applied magnetic field. When the catalyst was reused, the removal efficiency of 2,4-DCP was almost 100% for the first seven uses, and gradually decreased to 75% in cycles 8–10. Therefore, the Ni/Fe–Fe_3O_4 nanocomposites can be considered as a potentially effective tool for remediation of pollution by 2,4-DCP. 相似文献
13.
Alejandro Bermejo-López Be?at Pereda-Ayo Jon A.Onrubia-Calvo JoséA.González-Marcos Juan R.González-Velasco 《环境科学学报(英文版)》2024,(6):292-305
Integrated CO2capture and utilization (ICCU) technology requires dual functional materials(DFMs) to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na2CO3-8%CaO/γ-Al2O3DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static a... 相似文献
14.
The photocatalytic oxidation of gaseous chlorobenzene(CB) by the 365 nm-induced photocatalyst La/N–Ti O2, synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology(RSM) was used to model and optimize the conditions for synthesis of the photocatalyst. The optimal photocatalyst was 1.2La/0.5N–Ti O2(0.5) and the effects of La/N on crystalline structure, particle morphology, surface element content, and other structural characteristics were investigated by XRD(X-ray diffraction), TEM(Transmission Electron Microscopy), FTIR(Fourier transform infrared spectroscopy), UV–vis(Ultraviolet–visible spectroscopy), and BET(Brunauer Emmett Teller). Greater surface area and smaller particle size were produced with the co-doped Ti O2 nanotubes than with reference Ti O2. The removal of CB was effective when performed using the synthesized photocatalyst,though it was less efficient at higher initial CB concentrations. Various modified Langmuir-Hinshelwood kinetic models involving the adsorption of chlorobenzene and water on different active sites were evaluated. Fitting results suggested that competitive adsorption caused by water molecules could not be neglected, especially for environments with high relative humidity. The reaction intermediates found after GC–MS(Gas chromatography–mass spectrometry) analysis indicated that most were soluble, low-toxicity, or both. The results demonstrated that the prepared photocatalyst had high activity for VOC(volatile organic compounds) conversion and may be used as a pretreatment prior to biopurification. 相似文献
15.
Particles and porous tablets based on Fe0/ZSM-5 composites prepared by ball-milling for heavy metals removal: Dissolved Fe2 +, pH, and mechanism 总被引:1,自引:0,他引:1
Novel, low-cost Fe~0/ZSM-5-based particles and porous tablets were prepared by a ballmilling method and used for the removal of Pb~(2+) in solution. Solid-phase characterization by scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy(SEMEDS) and transmission electron microscopy(TEM) revealed that the Fe0 microparticles were evenly loaded and tightly immobilized on the surface of ZSM-5 because of the extrusion/welding impact during ball-milling. For different Pb~(2+) concentrations, batch experiments indicated that the removal of Pb~(2+) increased with the decline of dissolved Fe2+and p H value in the solution for particles; opposite results were obtained for the tablets. The differences in the contact between both materials and Pb~(2+) were the main factor controlling Pb~(2+) removal in the solution. Investigation into the effect of initial p H value revealed that high p H reduced the number of electrons released from Fe corrosion. Consequently, low levels of removed Pb~(2+) and dissolved Fe~(2+) were synchronously observed. Also, simulated electroplating wastewater was treated using the prepared particles and porous tablets,and the removal order of Pb~(2+) Cr~(6+) Cu~(2+)≈ Cd~(2+) was observed. The Fe~0/ZSM-5 particles and tablets prepared through ball-milling show potential as materials for treatment of Pb~(2+) and other toxic metals. 相似文献
16.
Mehdi Hassanshahian Zeynab Bayat Simone Cappello Francesco Smedile Michail Yakimov 《环境科学学报(英文版)》2016,28(5):136-146
In order to better understand the effects of biostimulation and bioaugmentation processes on a marine microbial community, three different mesocosm experiments were planned. Natural seawater(10.000 L) was artificially polluted with crude oil(1 L) and(1) inorganic nutrients(Biostimulating Mesocosm, BM),(2) inorganic nutrients and an inoculum of Alcanivorax borkumensis SK2(Single Bioaugmentation Mesocosm, SBM),(3) inorganic nutrients and inoculums of A. borkumensis SK2 and Thalassolituus oleivorans MIL-1(Consortium Bioaugmentation Mesocosm, CBM). During the experimental period(20 days), samples were taken from each mesocosm and the community structure was analyzed by PCR–DGGE. The 16 S r RNA gene DGGE banding patterns and sequence analysis demonstrated that biostimulation had the lowest effect on microbial biodiversity in the mesocosms; however, the biodiversity of the marine microbial community dramatically decreased in the CBM(Shannon index was 0.6 in T3). The community structures among the three mesocosms were also markedly different,and major bacteria derived from DGGE bands were related to uncultured Gamma Proteobacteria. The biodegradation results show that the Single Bioaugmentation Mesocosm(SBM) system had the highest percentage of degradation(95%) in comparison to the BM mesocosm(80%) and CBM(70%). 相似文献
17.
Xueyong Zhou 《环境科学学报(英文版)》2020,32(4):409-410
正In the paper entitled Efficient adsorption of Mn(Ⅱ) by layered double hydroxides intercalated with di ethylenetriaminepentaacetic acid and the mechanistic study in Journal of Environmental Sciences,volume 85,page 56-65,there were problems with mathematical notation and dimensional errors in the calculation for Giibbs free energy.In Section 2.5:Adsorption isotherms and thermodynamics studies,authors calculated the Gibbs free energy change (△G°) 相似文献
18.
Transition metal iron and persistent free radicals(PFRs) both affect the redox properties of biochar, but the electron transfer relationship between them and the coupling reduction mechanism of Cr(Ⅵ) requires further investigation. To untangle the interplay between iron and PFRs in biochar and the infuences on redox properties, FeCl3-modified rice husk biochar(FBCs) was prepared and its reduction mechanism for Cr(Ⅵ) without light was evaluated. The FBCs had higher surface positive cha... 相似文献
19.
Jianrui Niu Haobin Liu Hengli Qian Jie Liu Mengyuan M Erhong Duan Lei Yu 《环境科学学报(英文版)》2020,32(2):260-272
In order to study their synergistic catalytic effects in toluene degradation, CuMn_2O_4/HTS-1(HTS-1 was a titanium silicon molecular sieve), Cu_(0.7)Mn_2Y_(0.3)O_x/HTS-1 and Cu_(0.7)Mn_2Ce_(0.3)O_x/HTS-1 catalysts were prepared by the impregnation method.The textural properties, redox properties and acidity of the catalysts were characterized by X-ray diffractometer(XRD),transmission electron microscopy(TEM), scanning electron microscopy(SEM), H_2 temperature-programmed reduction(H_2-TPR), X-ray photoelectron spectroscopy(XPS),frustrated total internal reflection(FT-IR), ammonium temperature-programmed desorption(NH_3-TPD) and pyridine adsorption internal reflection(Py-IR) measurements.The potential roles of Lewis acid sites(activating dioxygen) were discussed, and the experimental results indicated that the most efficient route for toluene degradation over Cu_(0.7)Mn_2Ce_(0.3)O_x/HTS-1(toluene conversion rate of 90%(T99) = 295℃) was ascribed to regulation of the synergistic effects of redox properties(activating molecular toluene) and Lewis acid sites(activating dioxygen).The Mars–Van–Krevelen(MVK) model was adopted to describe the reaction process of toluene oxidation, which gave an in-depth view into the toluene degradation over CuMn_2O_4/HTS-1, Cu_(0.7)Mn_2Y_(0.3)O_x/HTS-1 and Cu_(0.7)Mn_2Ce_(0.3)O_x/HTS-1.In addition, the synergistic effects between redox properties and Lewis acid sites were studied in detail. 相似文献