Polyferric silicate sulfate （PFSS） with high concentration was prepared using the composite-poly method. The coagulation properties and mechanisms of this new complex were probed using TEM, Fe-Ferron timed complex-c...Polyferric silicate sulfate （PFSS） with high concentration was prepared using the composite-poly method. The coagulation properties and mechanisms of this new complex were probed using TEM, Fe-Ferron timed complex-colorimetric method, and infrared spectrum method. The results showed that the flocculating effect of polyferric silicate sulfate had an advantage over polyferric sulfate （PFS）, as the optimum coagulation effect could be obtained when the Si/Fe mole ratio was 0.75 in accordance with its macrostructure of PFSS. According to the Fe-Ferron timed complex-colorimetric method, the Si species was mainly Sic, whereas, the Fe species were Fea and Fec in the copolymerization system. The infrared spectra indicated that the structure of these new flocculants was formed by polymers, mainly by olation, which was different from polyferric sulfate, and the vibration of M-OH-M of around 1100 cm^-1, also proved that there existed Fe-OH-Fe and its polymers in some forms.展开更多
The fractal dimensions in different topological spaces of polyferric chloride-humic acid （PFC-HA） flocs, formed in flocculating different kinds of humic acids （HA） water at different initial pH （9.0, 7.0, 5.0） a...The fractal dimensions in different topological spaces of polyferric chloride-humic acid （PFC-HA） flocs, formed in flocculating different kinds of humic acids （HA） water at different initial pH （9.0, 7.0, 5.0） and PFC dosages, were calculated by effective densitymaximum diameter, image analysis, and N2 absorption-desorption methods, respectively. The mass fractal dimensions （De） of PFC-HA floes were calculated by bi-logarithm relation of effective density with maximum diameter and Logan empirical equation. The Df value was more than 2.0 at initial pH of 7,0, which was 11% and 13% higher than those at pH 9.0 and 5.0, respecively, indicating the most compact flocs formed in flocculated HA water at initial pH of 7.0. The image analysis for those flocs indicates that after flocculating the HA water at initial pH greater than 7.0 with PFC flocculant, the fractal dimensions of D2 （logA vs. logdL） and D3 （logVsphere vs. logdL） of PFC-HA floes decreased with the increase of PFC dosages, and PFC-HA floes showed a gradually looser structure. At the optimum dosage of PFC, the D2 （logA vs. logdL） values of the flocs show 14%-43% difference with their corresponding Dr, and they even had different tendency with the change of initial pH values. However, the D2 values of the floes formed at three different initial pH in HA solution had a same tendency with the corresponding Df. Based on fractal Frenkel-Halsey-HiU （FHH） adsorption and desorption equations, the pore surface fractal dimensions （Ds） for dried powders of PFC-HA flocs formed in HA water with initial pH 9.0 and 7.0 were all close to 2.9421, and the Ds values of flocs formed at initial pH 5.0 were less than 2.3746. It indicated that the pore surface fractal dimensions of PFC-HA floes dried powder mainly show the irregularity from the mesopore-size distribution and marcopore-size distribution.展开更多
The oxidation rate of ferrous sulfate was investigated in the preparation of polyferric sulfate(PFS) coagulant. It was proved that this reaction is zero order with respect to Fe2+, first order with respect to NO2(g) a...The oxidation rate of ferrous sulfate was investigated in the preparation of polyferric sulfate(PFS) coagulant. It was proved that this reaction is zero order with respect to Fe2+, first order with respect to NO2(g) and first order with respect to the interface area between gas phase and liquid phase. If the partial pressure of NO2(g) in gas phase is increased or the interface area is increased, the time needed to complete the reaction will be decreased.展开更多
A crystalline polyferric sulfate(PFS) adsorbent was synthesized by oxidizing and precipitating ferrous ions in air atmospheric conditions. The morphology, structure, specific surface area(SSA), and adsorptive efficacy...A crystalline polyferric sulfate(PFS) adsorbent was synthesized by oxidizing and precipitating ferrous ions in air atmospheric conditions. The morphology, structure, specific surface area(SSA), and adsorptive efficacy of the adsorbent to As(Ⅲ) were characterized by scanning electron microscope(SEM) and transmission electron microscopy(TEM) images, X-ray diffraction(XRD) patterns, Fourier-transform infrared(FTIR) spectra, BET SSA analyses, and adsorption experiments. The adsorbent showed a near-spherical aggregate structure and had good crystallinity. A significant amount of α-goethite co-precipitated with PFS in the case of the initial ferrous concentration of 1 mol/L and increased SSA of the adsorbent. The stability region of ferric compounds in the process was drawn and applied to analyze the iron behavior during the synthesis. The adsorption of As(Ⅲ) in high As(Ⅲ)-containing solutions fitted the Langmuir isotherm model adequately. The absorbent with co-precipitation of α-goethite showed good adsorbability for As(Ⅲ) and good filtering performance in the high As(Ⅲ)-containing solution of 10–100 mg/L under acidic, neutral, and alkaline conditions(pH 2.09–9.01). After the adsorption process, the stability of the residues bearing As(Ⅲ) was evaluated by toxic characteristic leaching procedure(TCLP) tests. The results indicated that the residues were extremely stable, and the concentrations of arsenic in the leaching solutions were less than 0.01 mg/L.展开更多
Elevated arsenic（As） in groundwater poses a great threat to human health. Coagulation using mono- and poly-Fe salts is becoming one of the most cost-effective processes for groundwater As removal. However, a limitat...Elevated arsenic（As） in groundwater poses a great threat to human health. Coagulation using mono- and poly-Fe salts is becoming one of the most cost-effective processes for groundwater As removal. However, a limitation comes from insufficient understanding of the As removal mechanism from groundwater matrices in the coagulation process, which is critical for groundwater treatment and residual solid disposal. Here, we overcame this hurdle by utilizing microscopic techniques to explore molecular As surface complexes on the freshly formed Fe flocs and compared ferric（III） sulfate（FS） and polyferric sulfate（PFS）performance, and finally provided a practical solution in As-geogenic areas. FS and PFS exhibited a similar As removal efficiency in coagulation and coagulation/filtration in a two-bucket system using 5 mg/L Ca（ClO）_2. By using the two-bucket system combining coagulation and sand filtration, 500 L of As-safe water（〈 10 μg/L） was achieved during five treatment cycles by washing the sand layer after each cycle. Fe k-edge X-ray absorption near-edge structure（XANES） and As k-edge extended X-ray absorption fine structure（EXAFS） analysis of the solid residue indicated that As formed a bidentate binuclear complex on ferrihydrite, with no observation of scorodite or poorly-crystalline ferric arsenate. Such a stable surface complex is beneficial for As immobilization in the solid residue, as confirmed by the achievement of much lower leachate As（0.9 μg/L-0.487 mg/L）than the US EPA regulatory limit（5 mg/L）. Finally, PFS is superior to FS because of its lower dose, much lower solid residue, and lower cost for As-safe drinking water.展开更多
Polyferric\|silicate\|sulfate(PFSS),as a new type of coagulant,was prepared by using sodium silicate, sulfuric acid and ferric sulfate as materials.The zeta potential of hydrolyzate of PFSS under different pH values w...Polyferric\|silicate\|sulfate(PFSS),as a new type of coagulant,was prepared by using sodium silicate, sulfuric acid and ferric sulfate as materials.The zeta potential of hydrolyzate of PFSS under different pH values was investigated.The effects of Fe/SiO\-2 molar ratio and dosage of PFSS on turbidity removal were studied. The relation between the optimum coagulation pH range and Fe/SiO\-2 molar ratio was found and the coagulation mechanism of PFSS was discussed.The experimental results showed that Fe/SiO\-2 molar ratio has an effect on the zeta potential of hydrolyzate, the coagulation performance and the optimum coagulation pH range of PFSS and that PFSS gives the best turbidity removal effect when its Fe/SiO\-2 molar ratio was 1.5.展开更多
Coagulation-flocculation process was applied in the pretreatment of diosgenin wastewater.Polyferric sulfate was used as primary coagulant and a cationic polyacrylamide （CPAM） was used as coagulant aid.Using jar test...Coagulation-flocculation process was applied in the pretreatment of diosgenin wastewater.Polyferric sulfate was used as primary coagulant and a cationic polyacrylamide （CPAM） was used as coagulant aid.Using jar test procedure,the influence of the main operating parameters,such as effluent pH and coagulant dosage in the coagulation performance was investigated.The effective pH was found to be in the range of 6.5-8.0 and coagulant dosage was 100 mg/L.Under the optimal conditions,15% chemical oxygen demand （COD） removal efficiency was achieved and the residual turbidity was less than 20 NTU.The presence of CPAM substantially promoted the reduction of residual turbidity with the appropriate CPAM dosage in the range of 2-5 mg/L.展开更多
The oxidation rate of ferrous sulfate is investigated for the preparation of polyferric sulfate(PFS) coagulant. It is proved that this reaction is zero order with respect to Fe 2+ , first order with respect to NO ...The oxidation rate of ferrous sulfate is investigated for the preparation of polyferric sulfate(PFS) coagulant. It is proved that this reaction is zero order with respect to Fe 2+ , first order with respect to NO 2(g), and first order with respect to the interface area between gas phase and liquid phase. According to this mechanism, sectionalized reactor(SR) is used in place of traditional reactor(TR), and the liquid of reaction mixture is recycled by pump. As a result, not only the flow path of reaction liquid is prolonged, but also gas liquid contact area enlarged, and the reaction distinctly accelerated, compared with traditional reactor. The effects of parameters including temperature, acidity and others on the reaction rate are also discussed.展开更多
Vivianite is often found in reducing environments rich in iron and phosphorus from organic debris degradation or phosphorus mineral dissolution. The formation of vivianite is essential to the geochemical cycling of ph...Vivianite is often found in reducing environments rich in iron and phosphorus from organic debris degradation or phosphorus mineral dissolution. The formation of vivianite is essential to the geochemical cycling of phosphorus and iron elements in natural environments. In this study, extracellular polymeric substances(EPS) were selected as the source of phosphorus. Microcosm experiments were conducted to test the evolution of mineralogy during the reduction of polyferric sulfate flocs(PFS) by Shewanella oneidensis MR-1(S. oneidensis MR-1) at EPS concentrations of 0, 0.03, and 0.3 g/L. Vivianite was found to be the secondary mineral in EPS treatment when there was no phosphate in the media. The EPS DNA served as the phosphorus source and DNA-supplied phosphate could induce the formation of vivianite.EPS impedes PFS aggregation, contains redox proteins and stores electron shuttle, and thus greatly promotes the formation of minerals and enhances the reduction of Fe(Ⅲ). At EPS concentration of 0, 0.03, and 0.3 g/L, the produced HCl-extractable Fe(Ⅱ) was 107.9, 111.0,and 115.2 mg/L, respectively. However, when the microcosms remained unstirred, vivianite can be formed without the addition of EPS. In unstirred systems, the EPS secreted by S. oneidensis MR-1 could agglomerate at some areas, resulting in the formation of vivianite in the proximity of microbial cells. It was found that vivianite can be generated biogenetically by S. oneidensis MR-1 strain and EPS may play a key role in iron reduction and concentrating phosphorus in the oligotrophic ecosystems where quiescent conditions prevail.展开更多
文摘Polyferric silicate sulfate （PFSS） with high concentration was prepared using the composite-poly method. The coagulation properties and mechanisms of this new complex were probed using TEM, Fe-Ferron timed complex-colorimetric method, and infrared spectrum method. The results showed that the flocculating effect of polyferric silicate sulfate had an advantage over polyferric sulfate （PFS）, as the optimum coagulation effect could be obtained when the Si/Fe mole ratio was 0.75 in accordance with its macrostructure of PFSS. According to the Fe-Ferron timed complex-colorimetric method, the Si species was mainly Sic, whereas, the Fe species were Fea and Fec in the copolymerization system. The infrared spectra indicated that the structure of these new flocculants was formed by polymers, mainly by olation, which was different from polyferric sulfate, and the vibration of M-OH-M of around 1100 cm^-1, also proved that there existed Fe-OH-Fe and its polymers in some forms.
基金supported by the National Natural Science Foundation of China (No. 20407004, 50578012, 50178009)the High-Tech Research and Development Program (863) of China (No. 2007AA06Z301)+2 种基金the Fok Ying Tung Education Foundation of National Education Ministry of China (No. 91078)the Beijing Municipal Commission of Education Project, Program for New Cen- tury Excellent Talents in University (No. NCET-06-0120)the Beijing Nova of Science and Technology, Beijing Key Subject (No. XK100220555).
文摘The fractal dimensions in different topological spaces of polyferric chloride-humic acid （PFC-HA） flocs, formed in flocculating different kinds of humic acids （HA） water at different initial pH （9.0, 7.0, 5.0） and PFC dosages, were calculated by effective densitymaximum diameter, image analysis, and N2 absorption-desorption methods, respectively. The mass fractal dimensions （De） of PFC-HA floes were calculated by bi-logarithm relation of effective density with maximum diameter and Logan empirical equation. The Df value was more than 2.0 at initial pH of 7,0, which was 11% and 13% higher than those at pH 9.0 and 5.0, respecively, indicating the most compact flocs formed in flocculated HA water at initial pH of 7.0. The image analysis for those flocs indicates that after flocculating the HA water at initial pH greater than 7.0 with PFC flocculant, the fractal dimensions of D2 （logA vs. logdL） and D3 （logVsphere vs. logdL） of PFC-HA floes decreased with the increase of PFC dosages, and PFC-HA floes showed a gradually looser structure. At the optimum dosage of PFC, the D2 （logA vs. logdL） values of the flocs show 14%-43% difference with their corresponding Dr, and they even had different tendency with the change of initial pH values. However, the D2 values of the floes formed at three different initial pH in HA solution had a same tendency with the corresponding Df. Based on fractal Frenkel-Halsey-HiU （FHH） adsorption and desorption equations, the pore surface fractal dimensions （Ds） for dried powders of PFC-HA flocs formed in HA water with initial pH 9.0 and 7.0 were all close to 2.9421, and the Ds values of flocs formed at initial pH 5.0 were less than 2.3746. It indicated that the pore surface fractal dimensions of PFC-HA floes dried powder mainly show the irregularity from the mesopore-size distribution and marcopore-size distribution.
文摘The oxidation rate of ferrous sulfate was investigated in the preparation of polyferric sulfate(PFS) coagulant. It was proved that this reaction is zero order with respect to Fe2+, first order with respect to NO2(g) and first order with respect to the interface area between gas phase and liquid phase. If the partial pressure of NO2(g) in gas phase is increased or the interface area is increased, the time needed to complete the reaction will be decreased.
基金financially supported by the National Natural Science Foundation of China(No.51574285)
文摘A crystalline polyferric sulfate(PFS) adsorbent was synthesized by oxidizing and precipitating ferrous ions in air atmospheric conditions. The morphology, structure, specific surface area(SSA), and adsorptive efficacy of the adsorbent to As(Ⅲ) were characterized by scanning electron microscope(SEM) and transmission electron microscopy(TEM) images, X-ray diffraction(XRD) patterns, Fourier-transform infrared(FTIR) spectra, BET SSA analyses, and adsorption experiments. The adsorbent showed a near-spherical aggregate structure and had good crystallinity. A significant amount of α-goethite co-precipitated with PFS in the case of the initial ferrous concentration of 1 mol/L and increased SSA of the adsorbent. The stability region of ferric compounds in the process was drawn and applied to analyze the iron behavior during the synthesis. The adsorption of As(Ⅲ) in high As(Ⅲ)-containing solutions fitted the Langmuir isotherm model adequately. The absorbent with co-precipitation of α-goethite showed good adsorbability for As(Ⅲ) and good filtering performance in the high As(Ⅲ)-containing solution of 10–100 mg/L under acidic, neutral, and alkaline conditions(pH 2.09–9.01). After the adsorption process, the stability of the residues bearing As(Ⅲ) was evaluated by toxic characteristic leaching procedure(TCLP) tests. The results indicated that the residues were extremely stable, and the concentrations of arsenic in the leaching solutions were less than 0.01 mg/L.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB14020201)the National Natural Science Foundation of China (Nos. 41373123, 21337004)the Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences (No. YSW2013A01)
文摘Elevated arsenic（As） in groundwater poses a great threat to human health. Coagulation using mono- and poly-Fe salts is becoming one of the most cost-effective processes for groundwater As removal. However, a limitation comes from insufficient understanding of the As removal mechanism from groundwater matrices in the coagulation process, which is critical for groundwater treatment and residual solid disposal. Here, we overcame this hurdle by utilizing microscopic techniques to explore molecular As surface complexes on the freshly formed Fe flocs and compared ferric（III） sulfate（FS） and polyferric sulfate（PFS）performance, and finally provided a practical solution in As-geogenic areas. FS and PFS exhibited a similar As removal efficiency in coagulation and coagulation/filtration in a two-bucket system using 5 mg/L Ca（ClO）_2. By using the two-bucket system combining coagulation and sand filtration, 500 L of As-safe water（〈 10 μg/L） was achieved during five treatment cycles by washing the sand layer after each cycle. Fe k-edge X-ray absorption near-edge structure（XANES） and As k-edge extended X-ray absorption fine structure（EXAFS） analysis of the solid residue indicated that As formed a bidentate binuclear complex on ferrihydrite, with no observation of scorodite or poorly-crystalline ferric arsenate. Such a stable surface complex is beneficial for As immobilization in the solid residue, as confirmed by the achievement of much lower leachate As（0.9 μg/L-0.487 mg/L）than the US EPA regulatory limit（5 mg/L）. Finally, PFS is superior to FS because of its lower dose, much lower solid residue, and lower cost for As-safe drinking water.
文摘Polyferric\|silicate\|sulfate(PFSS),as a new type of coagulant,was prepared by using sodium silicate, sulfuric acid and ferric sulfate as materials.The zeta potential of hydrolyzate of PFSS under different pH values was investigated.The effects of Fe/SiO\-2 molar ratio and dosage of PFSS on turbidity removal were studied. The relation between the optimum coagulation pH range and Fe/SiO\-2 molar ratio was found and the coagulation mechanism of PFSS was discussed.The experimental results showed that Fe/SiO\-2 molar ratio has an effect on the zeta potential of hydrolyzate, the coagulation performance and the optimum coagulation pH range of PFSS and that PFSS gives the best turbidity removal effect when its Fe/SiO\-2 molar ratio was 1.5.
基金supported by the National Natural Science Foundation of China (No. 40830748)China Postdoctoral Science Foundation (No. 20080440976)
文摘Coagulation-flocculation process was applied in the pretreatment of diosgenin wastewater.Polyferric sulfate was used as primary coagulant and a cationic polyacrylamide （CPAM） was used as coagulant aid.Using jar test procedure,the influence of the main operating parameters,such as effluent pH and coagulant dosage in the coagulation performance was investigated.The effective pH was found to be in the range of 6.5-8.0 and coagulant dosage was 100 mg/L.Under the optimal conditions,15% chemical oxygen demand （COD） removal efficiency was achieved and the residual turbidity was less than 20 NTU.The presence of CPAM substantially promoted the reduction of residual turbidity with the appropriate CPAM dosage in the range of 2-5 mg/L.
文摘The oxidation rate of ferrous sulfate is investigated for the preparation of polyferric sulfate(PFS) coagulant. It is proved that this reaction is zero order with respect to Fe 2+ , first order with respect to NO 2(g), and first order with respect to the interface area between gas phase and liquid phase. According to this mechanism, sectionalized reactor(SR) is used in place of traditional reactor(TR), and the liquid of reaction mixture is recycled by pump. As a result, not only the flow path of reaction liquid is prolonged, but also gas liquid contact area enlarged, and the reaction distinctly accelerated, compared with traditional reactor. The effects of parameters including temperature, acidity and others on the reaction rate are also discussed.
基金supported by the National Natural Science Foundation of China (No. 41673090)the Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control (No. 2017B030301012)the Local Innovation and Entrepreneurship Team Project of Guangdong Special Support Program (No. 2019BT02L218)。
文摘Vivianite is often found in reducing environments rich in iron and phosphorus from organic debris degradation or phosphorus mineral dissolution. The formation of vivianite is essential to the geochemical cycling of phosphorus and iron elements in natural environments. In this study, extracellular polymeric substances(EPS) were selected as the source of phosphorus. Microcosm experiments were conducted to test the evolution of mineralogy during the reduction of polyferric sulfate flocs(PFS) by Shewanella oneidensis MR-1(S. oneidensis MR-1) at EPS concentrations of 0, 0.03, and 0.3 g/L. Vivianite was found to be the secondary mineral in EPS treatment when there was no phosphate in the media. The EPS DNA served as the phosphorus source and DNA-supplied phosphate could induce the formation of vivianite.EPS impedes PFS aggregation, contains redox proteins and stores electron shuttle, and thus greatly promotes the formation of minerals and enhances the reduction of Fe(Ⅲ). At EPS concentration of 0, 0.03, and 0.3 g/L, the produced HCl-extractable Fe(Ⅱ) was 107.9, 111.0,and 115.2 mg/L, respectively. However, when the microcosms remained unstirred, vivianite can be formed without the addition of EPS. In unstirred systems, the EPS secreted by S. oneidensis MR-1 could agglomerate at some areas, resulting in the formation of vivianite in the proximity of microbial cells. It was found that vivianite can be generated biogenetically by S. oneidensis MR-1 strain and EPS may play a key role in iron reduction and concentrating phosphorus in the oligotrophic ecosystems where quiescent conditions prevail.
