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1.
The removal efficiency of copper(Cu(Ⅱ)) from an actual acidic electroplating effluent by biochars generated from canola,rice,soybean and peanut straws was investigated.The biochars simultaneously removed Cu(Ⅱ) from the effluent,mainly through the mechanisms of adsorption and precipitation,and neutralized its acidity.The removal efficiency of Cu(Ⅱ) by the biochars followed the order:peanut straw char > soybean straw char > canola straw char > rice straw char a commercial activated carbonaceous material,which is consistent with the alkalinity of the biochars.The pH of the effluent was a key factor determining the removal efficiency of Cu(Ⅱ) by biochars.Raising the initial pH of the effluent enhanced the removal of Cu(Ⅱ) from it.The optimum pyrolysis temperature was 400°C for producing biochar from crop straws for acidic wastewater treatment,and the optimum reaction time was 8 hr.  相似文献   

2.
The study was to investigate the adsorption behavior of arsenite (As(Ⅲ)) and arsenate (As(Ⅴ)) on two variable charge soils, i.e., Haplic Acrisol and Rhodic Ferralsol at different ionic strengths and pH with batch methods. Results indicated that the amount of As(Ⅲ) adsorbed by these two soils increased with increasing solution pH, whereas it decreased with increasing ionic strength under the acidic condition. This suggested that As(Ⅲ) was mainly adsorbed on soil positive charge sites through electrostatic attraction under the acidic condition. Moreover, intersects of As(Ⅴ) adsorption-pH curves at different ionic strengths (a characteristic pH) are obtained for both soils. It was noted that above this pH, the adsorption of As(Ⅴ) was increased with increasing ionic strength, whereas below it the reverse trend was true. Precisely the intersect pH was 3.6 for Haplic Acrisol and 4.5 for Rhodic Ferralsol, which was near the values of PZSE (soil point of zero salt effect) of these soils. The effects of ionic strength and pH on arsenate adsorption by these soils were interpreted by the adsorption model. The results of zeta potential suggested that the potential in adsorption plane becomes less negative with increasing ionic strength above soil PZSE and decreases with increasing ionic strength below soil PZSE. These results further supported the hypothesis of the adsorption model that the potential in the adsorption plane changes with ionic strength with an opposite trend to surface charge of the soils. Therefore, the change of the potential in the adsorption plane was mainly responsible for the change of arsenate adsorption induced by ionic strength on variable charge soils.  相似文献   

3.
Loofa sponge (LS) immobilized biomass of Chlorella sorokiniana (LSIBCS), isolated from industrial wastewater, was investigated as a new biosorbent for the removal of Cr(Ⅲ) from aqueous solution. A comparison of the biosorption of Cr(Ⅲ) by LSIBCS and free biomass of C. sorokiniana (FBCS) from 10-300 mg Cr(Ⅲ)/L aqueous solutions showed an increase in uptake of 17.79% when the microalgal biomass was immobilized onto loofa sponge. Maximum biosorption capacity for LSIBCS and FBCS was found to be 69.26 and 58.80 mg Cr(Ⅲ)/g biosorbent, respectively, whereas the amount of Cr(Ⅲ) ions adsorbed onto naked LS was 4.97 mg/g. The kinetics of Cr(Ⅲ) biosorption was extremely rapid and equilibrium was established in about 15 and 20 min by LSIBCS and FBCS, respectively. The biosorption equilibrium was well defined by Langmuir adsorption isotherm model. The biosorption kinetics followed the pseudo-second order kinetic model. The biosorption was found to be pH dependent and the maximum sorption occurred at the solution pH 4.0. Desorption studies showed that 98% of the adsorbed Cr(Ⅲ) could be desorbed with 0.1 mol/L HNO3, while other desorbing agents were less effective in the order: EDTA 〉 H2SO4 〉 CH3COOH 〉 HCl. The regenerated LSIBCS retained 92.68% of the initial Cr(Ⅲ) binding capacity up to five cycles of reuse in continuous flow-fixed bed columns. The study revealed that LSIBCS could be used as an effective biosorbent for the removal of Cr(Ⅲ) from wastewater.  相似文献   

4.
Pollutants that exist in anionic species are issues of concern in water treatment. Compared to cationic pollutants, the removal of anionic pollutants by adsorption is more difficult because most adsorbents carry predominantly negative charges in neutral and alkaline environments. In this study, a cross-linked chitosan derivative with quaternary ammonium and magnetic properties(QM-chitosan) was prepared and employed to remove chromium(VI) and phosphorus(V)(Cr(VI) and P(V)) from aqueous environments. The QM-chitosan was characterized by Fourier transform infrared spectrometry(FT-IR),thermogravimetric analysis(TGA), energy dispersive X-ray(SEM-EDX) and zeta potential.Batch experiments show that QM-chitosan can effectively remove Cr(VI) and P(V), and the main mechanism was believed to be electrostatic interaction. A pseudosecond-order model was fitted to describe the kinetic processes of Cr(VI) and P(V) removal. The adsorption isotherms of both Cr(VI) and P(V) on the QM-chitosan were well fitted by the Langmuir isotherm equation. The saturated adsorption capacity of P(V)(2.783 mmol/g) was found to be higher than that of Cr(VI)(2.323 mmol/g), resulting from the size of the H2PO-4ions being smaller than that of the HCr O-4ions. However, the theoretical calculation and experimental results showed that QM-chitosan had a stronger affinity for Cr(VI) than P(V). The adsorption–desorption of the QM-chitosan was evaluated, and high regeneration rates were demonstrated.  相似文献   

5.
Kinetics and isotherms of Neutral Red adsorption on peanut husk   总被引:2,自引:0,他引:2  
Adsorption of Neutral Red (NR) onto peanut husk in aqueous solutions was investigated at 295 K. Experiments were carried out as function of pH, adsorbent dosage, contact time, and initial concentration. The equilibrium adsorption data were analyzed by Langmuir, Freundlich, Temkin, Dubinin-Radushkevich, and Toth isotherm models. The results indicated that the Toth and Langmuir models provided the best correlation of the experimental data. The adsorption capacity of peanut husk for the removal of NR was deter...  相似文献   

6.
Due to their widespread use, clofibric acid (CA) and carbamazepine (CBZ) have been frequently detected simultaneously at relatively high concentrations in aquatic environments. In this study, agricultural waste rice straw was employed as a potentially low-cost, effective and easy-to-operate biosorbent (RSB) to remove CA and CBZ. The adsorption of both pharmaceuticals followed pseudo second-order kinetics, and intraparticle diffusion was an important rate-limiting step. The adsorption isotherms of both drugs were fit well with Freundlich model. The adsorption of CA onto RSB was exothermic and was more likely to be dominated by physical processes, while the adsorption of CBZ was endothermic. Solution pH was determined to be the most important factor for CA adsorption, such that the adsorption capacity of CA onto RSB increased with the decline of solution pH. In the lower range of solution pH below 3. l, the CA removal efficiency was enhanced with the increase of biosorbent dosage. The CBZ removal efficiency was enhanced with the increase of RSB dosage without pH control. The maximum adsorption capacities were 126.3 mg/g for CA and 40.0 mg/g for CBZ.  相似文献   

7.
Pyrolysis has the potential of transforming waste into valuable recyclable products. Pyrolytic char (PC) is one of the most important products from the pyrolysis of used tires. One of the most significant applications for pyrolytic char recovered is used for the removal of Cr( Ⅵ ) in the wastewater effluent to control waste by waste. The surface chemistry properties of surface element distribution/concentration and chemical structure were examined for the pyrolytic char and the commercial activated carbon(CAC) respectively. The results showed that surfaces of PC possesses a large amount of ester and hydrocarbon graft, whereas there are mainly carbon functional components of C-OH, C=O and COOH on the surface of CAC. Therefore the surface electronegativity of PC is lower than that of CAC in the water. The repulsive interactions between the surfaces of PC and the negatively charged Cr(Ⅵ ) ion are weaker than that of CAC,which results in an intensification of the adsorption process by the utilization of PC. The adsorption isotherms of Cr( Ⅵ ) ion on the two kinds of carbons were determined experimentally. The larger adsorption amount on the PC in the case of Cr( Ⅵ ) may be attributed mainly to its special surface micro-chemical environment. The mechanism of the removal Cr( Ⅵ ) from aqueous solution was assumed to be the integration of adsorption and redox reaction. The adsorption was the rate-controlled step for Cr( Ⅵ ) removal. The adsorption of Cr( Ⅵ )was identified as pseudo-second-order kinetics. The rate constants of adsorption were evaluated.  相似文献   

8.
Adsorption mechanisms and the role of different porous and crystalline structures on the removal of five haloacetonitriles (HANs) over hexagonal mesoporous silica (HMS), titanium substituted mesoporous silica (Ti-HMS), rod-shaped SBA-15 and microporous zeolite NaY were investigated. In addition, the effect of pH on adsorption mechanism and selective adsorption of five HANs individually and in an equimolar mixed solution were evaluated. The results indicated that the intraparticle diffusion rate constants of the mesoporous adsorbents were higher than that of the microporous NaY. In single solute, the order of adsorption preference (highest to lowest) was mono-HANs?>?di-HANs?>?tri-HAN. However, in mixed solute, the large molecular weight of the tri-HAN and di-HANs are more easily adsorbed than the smaller molecular weight mono-HANs. Except for SBA-15, the order of adsorption capacities in mixed HANs solute was not different compared to that observed for the single HAN solute, which might be caused by the higher accessibility to the active sites due to larger pore size. The ion-dipole electrostatic interaction was likely to be the main adsorption mechanism, and was favored at high pH values due to the high negative surface charge density of the adsorbent. The molecular structure of the HANs and hydrophilic/hydrophobic nature affected the adsorption capacities and their selective adsorption from mixed solutes.  相似文献   

9.
A novel amphoteric granular lignin adsorbent(AGLA) was prepared using magnesium lignosulfonate as a raw material which was provided by a straw sulfite pulp mill in Guangdong Province, China. A reactive dye(red K-3B) was used as an adsorbate to investigate the adsorption behavior by static and mobile ways. The removal of reactive red K-3B was found to be initially pH and concentration dependent.Moreover, an increase of solution temperature ranging from 5℃ to 60℃ helped to enhance the rate of intraparticle diffusion of adsorbate and changes in the size of the pores of the adsorbent and thus to reduce the adsorption time. The total breakthrough adsorption capacity was 531 mg/g, and the saturated adsorption capacity was 560 mg/g, which prevailed over the activated carbons evidently. The reactive red K-3B adsorbed on AGLA could be recovered with a mixture of alcohol, NaCI and HCI aqueous solutions. The recovery percentage could reach 92.4%.  相似文献   

10.
Loofa sponge (LS) immobilized biomass of Chlorella sorokiniana (LSIBCS), isolated from industrial wastewater, was investigated as a new biosorbent for the removal of Cr(Ⅲ) from aqueous solution. A comparison of the biosorption of Cr(Ⅲ) by LSIBCS and free biomass of C. sorokiniana (FBCS) from 10-300 mg Cr(Ⅲ)/L aqueous solutions showed an increase in uptake of 17.79% when the microalgal biomass was immobilized onto loofa sponge. Maximum biosorption capacity for LSIBCS and FBCS was found to be 69.26 and 58.80 mg Cr(Ⅲ)/g biosorbent, respectively, whereas the amount of Cr(Ⅲ) ions adsorbed onto naked LS was 4.97 mg/g. The kinetics of Cr(Ⅲ) biosorption was extremely rapid and equilibrium was established in about 15 and 20 min by LSIBCS and FBCS,respectively. The biosorption equilibrium was well defined by Langmuir adsorption isotherm model. The biosorption kinetics followed the pseudo-second order kinetic model. The biosorption was found to be pH dependent and the maximum sorption occurred at the solution pH 4.0. Desorption studies showed that 98% of the adsorbed Cr(Ⅲ) could be desorbed with 0.1 mol/L HNO3, while other desorbing agents were less effective in the order: EDTA > H2SO4 > CH3COOH > HCl. The regenerated LSIBCS retained 92.68% of the initial Cr(Ⅲ) binding capacity up to five cycles of reuse in continuous flow-fixed bed columns. The study revealed that LSIBCS could be used as an effective biosorbent for the removal of Cr(Ⅲ) from wastewater.  相似文献   

11.
Batch adsorption from aqueous solutions in a slightly basic medium of Methylene Blue, up to 2500 mg/L, onto synthetic magnesium silicate (Florisil) of three particle size ranges (mean diameters of 112, 200 and 425 μm) was compared to the corresponding adsorption onto activated carbon and Amberlite XAD-2. The best fit of the kinetic results was achieved by a pseudo second-order equation. The equilibrium data were found to be well represented by the Langmuir isotherm equation. Amberlite XAD-2, an unspecific adsorbent capable of adsorbing exclusively through a surface effect, exhibited a poor dye uptake, confirming that the adsorption mechanism on Florisil was due to electrostatic attraction and ion exchange. Moreover, the comparison between Florisil and the other adsorbents was performed on the basis of the evaluation of the surface area and pore volume occupied by the adsorbed dye.  相似文献   

12.
Adsorption behavior of condensed phosphate on aluminum hydroxide   总被引:1,自引:0,他引:1  
Sodium pyrophosphate (pyro-P, Na4P2OT), sodium tripolyphosphate (tripoly-P, Na3P3O10), and sodium hexametaphosphate (meta-P, (NaPO3)6) were selected as the model compounds of condensed phosphate to investigate the adsorption behavior of condensed phosphate on aluminum hydroxide. The adsorption was found to be endothermic and divisible into two stages: (1) fast adsorption within 1 h; and (2) slow adsorption between 1 and 24 h. The modified Freundlich model simulated the fast adsorption stage well; the slow adsorption stage was described well by the first-order kinetics. The activation energies of pyro-P, tripoly-P, and meta-P adsorption on aluminum hydroxide were determined to be 20.2, 22.8 and 10.9 kJ/mol P adsorbed, respectively, in the fast adsorption stage and to be 66.3, 53.5 and 72.5 kJ/mol P adsorbed, respectively, in the slow adsorption stage. The adsorption increased the negative charge of the aluminum hydroxide surface. Transmission electron microscopy and energy dispersive X-ray analysis analyses provided evidence that the adsorption was not uniform on the surface and that the small crystals contributed more to the fast adsorption than the normal sites did. The results from X-ray fluorescence spectrometry and X-ray photoelectron spectroscopy tests also revealed the uneven adsorption of condensed phosphate as a function of the penetration depth. More condensed phosphates were adsorbed on the outer surface of aluminum hydroxide than in its inner parts.  相似文献   

13.
The adsorption characteristics and mechanisms of the biosorbent from waste activated sludge were investigated by adsorbing Pb2+and Zn2+in aqueous single-metal solutions. A p H value of the metal solutions at 6.0 was beneficial to the high adsorption quantity of the biosorbent. The optimal mass ratio of the biosorbent to metal ions was found to be 2. A higher adsorption quantity of the biosorbent was achieved by keeping the reaction temperature below 55°C. Response surface methodology was applied to optimize the biosorption processes, and the developed mathematical equations showed high determination coefficients(above 0.99 for both metal ions) and insignificant lack of fit(p = 0.0838 and 0.0782 for Pb2+and Zn2+, respectively). Atomic force microscopy analyses suggested that the metal elements were adsorbed onto the biosorbent surface via electrostatic interaction. X-ray photoelectron spectroscopy analyses indicated the presence of complexation(between –NH2,-CN and metal ions) and ion-exchange(between –COOH and metal ions). The adsorption mechanisms could be the combined action of electrostatic interaction, complexation and ion-exchange between functional groups and metal ions.  相似文献   

14.
The adsorption characteristics of heavy metals: Cu(Ⅱ), Pb(Ⅱ), Zn(Ⅱ) and Cd(Ⅱ) ions on tourmaline were studied. Adsorption equilibrium was established. The adsorption isotherms of all the four metal ions followed well Langmuir equation. Tourmaline was found to remove heavy metal ions efficiently from aqueous solution with selectivity in the order of Pb(Ⅱ)〉Cu(Ⅱ)〉Cd(Ⅱ)〉Zn(Ⅱ). The adsorption of metal ions by tourmaline increased with the initial concentration of metal ions increasing in the medium. Tourmaline could also increase pH value of metal solution.The maximum heavy metal ions adsorbed by tourmaline was found to be 78.86, 154.08, 67.25, and 66.67 mg/g for Cu(Ⅱ), Pb(U), Zn(Ⅱ) and Cd(U), respectively. The temperature (25-55℃) had a small effect on the adsorption capacity of tourmaline. Competitive adsorption of Cu(Ⅱ), Pb(Ⅱ), Zn(Ⅱ) and Cd(Ⅱ) ions was also studied. The adsorption capacity of tourmaline for single metal decreased in the order of Pb〉Cu〉Zn 〉Cd and inhibition dominance observed in two metal systems was Pb〉Cu, Pb〉Zn, Pb〉Cd, Cu〉Zn, Cu〉Cd, and Cd〉Zn.  相似文献   

15.
A novel illite@carbon(I@C) nanocomposite adsorbent has been synthesized via a facile hydrothermal carbonization process(HTC) using glucose as carbonaceous source and illite as the carrier.The morphology,microstructure and surface properties of the prepared nanocomposite adsorbent were analyzed by FESEM,TGA,XRD,FT-IR and Zeta potential measurements.Batch experiments were carried out on the adsorption of Cr(Ⅵ) to determine the adsorption properties of the composite.The adsorption of Cr(Ⅵ) onto the I@C nanocomposite was well described by the pseudo-second-order kinetic model and Langmuir isotherm.Compared with the illite and carbon material(SC) separately,the prepared I@C nanocomposite adsorbent exhibited enhanced adsorption performance for Cr(Ⅵ) with a maximum adsorption capacity of 149.25 mg/g,which was higher than that of most reported adsorbents.In addition,the adsorption process was spontaneous and endothermic based on the adsorption thermodynamics study.The adsorption of Cr(Ⅵ) by I@C was highly p H-dependent and the optimum adsorption occurred at p H 2.0.The Zeta potential analysis results indicated that the electrostatic interactions between anionic Cr(Ⅵ) and the positively charged surface of the adsorbent might be critical to the adsorption mechanism.This study demonstrated that the I@C nanocomposite should be a promising candidate for a low-cost,environmental friendly and highly efficient adsorbent for the removal of toxic Cr(Ⅵ) from wastewater.  相似文献   

16.
Hexavalent chromium, Cr(VI), a highly toxic oxyanion known as a carcinogen and mutagen,is an issue of concern due to its adverse impact on human health. Therefore, development of effective technologies and/or materials for Cr(VI) removal from water has been of great interest for researchers. In this study, an electrospun carbon nanofiber(CNF) mat was prepared via electrospinning polyacrylonitrile(PAN), followed by thermal pre-oxidation and carbonization. Scanning electron microscopy(SEM) observation showed that the fiber diameter of the CNF with carbonization temperature of 950°C(CNF_(950)) was about 266 nm.Potentiometric titration analysis demonstrated that the point of zero charge p H(pHpzc) of CNF_(950) was around 7.93. CNF_(950) demonstrated high adsorption capacity and fast adsorption kinetics for Cr(VI) at pH 3. Langmuir isotherm calculations showed that the maximum adsorption capacity of Cr(VI) on CNF_(950) was 118.8 mg/g at pH 2. The adsorption isotherm of Cr(VI) on CNF_(950) was well described by the Redlich–Peterson model, revealing that Cr(VI)adsorption was the result of a combination of monolayer and multilayer adsorption,depending on the initial Cr(VI) concentration. Solution pH greatly affected Cr(VI) adsorption onto CNF_(950) due to the electrostatic interaction, and the adsorption capacity was relatively high when pH was below 3. X-ray photoelectron spectroscopy(XPS) analysis revealed that the removal of Cr(VI) might be the result of a combination of redox reaction and electrostatic adsorption. The adsorption-saturated CNF_(950) could be regenerated by NaOH solution. This study extends the potential applicability of electrospun CNF mats for Cr(VI)-contaminated water purification.  相似文献   

17.
Lagerstroemia speciosa bark(LB) embedded magnetic nanoparticles were prepared by co-precipitation of Fe~(2+) and Fe~(3+) salt solution with ammonia and LB for Cr(Ⅵ) removal from aqueous solution.The native LB,magnetic nanoparticle(MNP),L.spedosa embedded magnetic nanoparticle(MNPLB) and Cr(Ⅵ) adsorbed MNPLB particles were characterized by SEM-EDX,TEM,BET-surface area,FT-IR,XRD and TGA methods.TEM analysis confirmed nearly spherical shape of MNP with an average diameter of 8.76 nm and the surface modification did not result in the phase change of MNP as established by XRD analysis,while led to the formation of secondary particles of MNPLB with diameter of 18.54 nm.Characterization results revealed covalent binding between the hydroxyl group of MNP and carboxyl group of LB particles and further confirmed its physico-chemical nature favorable for Cr(Ⅵ) adsorption.The Cr(Ⅵ) adsorption on to MNPLB particle as an adsorbent was tested under different contact time,initial Cr(Ⅵ) concentration,adsorbent dose,initial pH,temperature and agitation speed.The results of the equilibrium and kinetics of adsorption were well described by Langmuir isotherm and pseudo-second-order model,respectively.The thermodynamic parameters suggest spontaneous and endothermic nature of Cr(Ⅵ)adsorption onto MNPLB.The maximum adsorption capacity for MNPLB was calculated to be 434.78 mg/g and these particles even after Cr(Ⅵ) adsorption were collected effortlessly from the aqueous solution by a magnet.The desorption of Cr(Ⅵ)-adsorbed MNPLB was found to be more than 93.72%with spent MNPLB depicting eleven successive adsorption-desorption cycles.  相似文献   

18.
Oxidation of As(Ⅲ) by potassium permanganate   总被引:2,自引:1,他引:2  
The oxidation of As(Ⅲ) with potassium permanganate was studied under conditions including pH, initial As(Ⅲ) concentration and dosage of Mn(Ⅶ). The results have shown that potassium permanganate was an effective agent for oxidation of As(Ⅲ) in a wide pH range. The pH value of tested water was not a significant factor affecting the oxidation of As(Ⅲ) by Mn(Ⅲ). Although theoretical redox analyses suggest that Mn(Ⅶ) should have better performance in oxidization of As(Ⅲ) within lower pH ranges, the experimental results show that the oxidation efficiencies of As(Ⅲ) under basic and acidic conditions were similar, which may be due to the adsorption of As(Ⅲ) on the Mn(OH)2 and MnO2 resulting from the oxidation of As(Ⅲ).  相似文献   

19.
The massive production and wide use of surfactants have resulted in a large amount of surfactant residuals being discharged into the environment,which could have an impact on arsenic behavior.In the present study,the influence of the anionic surfactant sodium dodecyl benzene sulfonate(SDBS) and nonionic surfactant polyethylene glycol octylphenyl ether(Triton X-100) on arsenic behavior was investigated in batch and column tests.The presence of SDBS and Triton X-100 reduced arsenic retention onto ferrihydrite(FH),enhanced arsenic transport through FH coated sand(FH-sand) columns and promoted arsenic release from the FH surface.With coexisting surfactants in solution,the equilibrium adsorbed amount of arsenic on FH decreased by up to 29.7% and the adsorption rate decreased by up to 52.3%.Pre-coating with surfactants caused a decrease in the adsorbed amount and adsorption rate of arsenic by up to 15.1% and 58.3%,respectively.Because of the adsorption attenuation caused by surfactants,breakthrough of As(Ⅴ) and As(Ⅲ) with SDBS in columns packed with FH-sand was 23.8% and 14.3%faster than that in those without SDBS,respectively.In columns packed with SDBS-coated FH-sand,transport of arsenic was enhanced to a greater extent.Breakthrough of As(Ⅴ) and As(Ⅲ) was 52.4% and 43.8% faster and the cumulative retention amount was 44.5% and 57.3% less than that in pure FH-sand column systems,respectively.Mobilization of arsenic by surfactants increased with the increase of the initial adsorbed amount of arsenic.The cumulative release amount of As(Ⅴ) and As(Ⅲ) from the packed column reached 10.8% and 36.0%,respectively.  相似文献   

20.
Two novel polymers (NJ-1 and N J-2) were synthesized by chemically modified a hypercrosslinked polymer NJ-0 with dimethylamine and trimethylamine, respectively. The comparison of the adsorption properties of the three polymers toward phenol, resorcin and phloroglucin was made. The study focused on the static equilibrium adsorption behaviors and the adsorption thermodynamics. Freundlich equation was found to fit the adsorption results well. The effect of amino groups introduced onto the surface of the resin and the structure of phenolic compounds on the adsorption were also studied. The hydrogen-bonding interaction and electrostatic interaction could happen between the amino groups and the adsorbates. The adsorption impetus increased as quantity of hydroxyl groups increased, but the adsorption capacity decreased due to the drop of the matching degree of the aperture of resins and the diameter of adsorbate molecules.  相似文献   

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