CN115386136B - Preparation method and application of aminated polyacrylamide foam adsorbent - Google Patents
Preparation method and application of aminated polyacrylamide foam adsorbent Download PDFInfo
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- C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
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Abstract
The invention discloses a preparation method and application of an aminated polyacrylamide foam adsorbent, wherein the preparation method of the aminated polyacrylamide foam adsorbent comprises the following steps: (1) Adding ammonium persulfate solution and tetramethyl ethylenediamine into the acrylamide and N-N methylene bisacrylamide monomer raw solution, introducing into a mold after rotation, sealing the liquid level, and obtaining polyacrylamide after reaction shaping; (2) Immersing polyacrylamide into a hydrochloric acid solution, adding aniline, then adding an ammonium persulfate solution, and immersing overnight to obtain an aminated polyacrylamide gel material; (3) And freeze-drying the obtained aminated polyacrylamide gel and firing to obtain the aminated polyacrylamide foam adsorbent. The adsorbent material prepared by the invention realizes the efficient selective adsorption removal of trace perfluorinated compounds in water through electrostatic adsorption and hydrophobic interaction and the formation of micelles in the adsorbent and semi-micelles on the surface of the adsorbent, and has low cost and is suitable for the pollution of trace perfluorinated compounds in drinking water.
Description
Technical Field
The invention belongs to the field of pollutant degradation, and particularly relates to a preparation method and application of an aminated polyacrylamide foam adsorbent.
Background
Perfluoro compounds (PFCs) are a novel class of organofluorides artificially synthesized at the end of the 40 th century, consisting of hydrophobic perfluoroalkyl chains and hydrophilic ion heads (Key B D, howell R D, criddle C S, et al, fluorinated organic in the biosphere environmental science&technical, 2007,31,2445-2454.Fujii S,Polprasert C,Tanaka S,et al.New POPs in the water environment:distribution,bioaccumulationand treatment of perfluorinated compounds-a review paper journal of Water Supply Research and Technology-aqua,2007,56,313-326. Because of their amphiphilic nature and high stability, they have been widely used in various industries since successful synthesis, such as textile, lubrication, surfactants, food packaging, non-stick coatings, electronics, fire-fighting foam, etc., causing serious environmental pollution (Lindstrom A B, strynar M J, delinsky A D, et al application of WWTP biosolids and resulting perfluorinated compound contamination of surface and well water in Decatur, alabama, USA. Environmental Science)&Technology,2011,45(19):8015-8021.Wang Z Y,DeWitt J C,Higgins C P,et al.A never-ending story of per-and polyfluoroalkyl substances(PFASs).Environmental Science&Technology,2017,51 (5): 2508-2518.). 2009In 2015, perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA) and salts thereof were successively listed in the persistent organic pollutant priority control list of the Stockholm convention, in 2016, the United states environmental protection agency EPA in turn prescribes that the health limiting concentration of PFOA and PFOS in drinking water be 70ng/L (Boone J S, vigo C, boone T, et al Per-and polyfluoroalkyl substances in source and treated drinking waters of the United states.science of the Total Environment,2019,653:359-369.Wang T,Wang Y W,Liao C Y,et al.Perspectives on the inclusion of perfluorooctane sulfonate into the stockholm convention on persistent organic pollutants.Environmental Science)&Technology,2009, 43:5171-5175.). Nevertheless, PFCs are highly thermally and chemically stable, persist in the environment, and are hardly biodegradable, resulting in still higher concentrations of PFCs in the environment (Liu Y, zhang Y, li J, et al distribution, partitioning behavior and positive matrix factorization-based source analysis of legacy and emerging polyfluorinated alkyl substances in the dissolved phase, surface sediment and suspended particulate matter around coastal areas of Bohai Bay, china. Environmental Pollution,2019, 246:34-44.). Research shows that PFCs in the environment enter human body mainly through drinking water, diet intake and other ways, and have certain organ, nerve, reproduction, immune toxicity and carcinogenicity. The use of PFOA and other PFCs with higher water solubility results in the most serious pollution of PFCs in water environment, so that drinking water becomes one of the most important ways for human ingestion of PFCs (Buck R C, franklin J, berger U, et al, perfluoylalkyl and polyfluoroalkyl substances in the environment: terminology, classification, and origins. Integrated Environmental Assessment and Management,2011,7 (4): 513-541.). The adsorption technology is widely applied to the removal of PFCs in water due to the advantages of simple operation, low energy consumption and the like, and the adsorbent commonly used at present mainly comprises activated carbon and ion exchange resin. However, in practical application, activated carbon has poor adsorption effect on hydrophobic and lipophobic PFCs, and ion exchange resin has the disadvantages of poor selectivity, high price, poor recycling property and the like (Sun M, zhou H, xu B, et al distribution) of perfluorinated compounds in drinking water treatment plant and reductive degradation by UV/SO 3 2 Process. Environmental Science and Pollution Research,2018,25 (8): 7443-7453.Yu Q,Zhang R Q,Deng S B,et al.Sorption of perfluorooctane sulfonate and perfluorooctanoate on activated carbons and resin:Kinetic and isotherm study.Water Research,2009,43 (4): 1150-1158.Maimaiti A,Deng S B,Meng P P,et al.Competitive adsorption of perfluoroalkyl substances on anion exchange resins in simulated AFFF-implemented group water. Chemical Engineering Journal,2018, 348:494-502.). In addition, the environment water contains different kinds of humus, salt ions and small molecular acid, and has great influence on the adsorption effect of the traditional material. Therefore, the development of a novel adsorbent which is low in cost and can efficiently and selectively remove PFCs is a key for treating PFCs polluted water.
In recent years, research has been conducted to focus on materials having aminated structures, and aminated adsorption materials have been expected to achieve selective adsorption of PFCs by increasing electrostatic adsorption of the materials to the PFCs through electron rearrangement effects (Klemes M J, ling Y H, ching C, et al reduction of a tetrafluoroterephthalonitrile-beta-cyclodextrin polymer to remove anionic micropollutants and perfluorinated alkyl substances from water. Angel process Chemie International Edition,2019,58 (35): 12049-12053.Kawano S,Kida T,Takemine S,et al.Efficient removal and recovery of perfluorinated compounds from water by surface-heated beta-cyclodextrins on polystyrene components chemistry Letters,2013,42 (4): 392-394.). As an organic polymer, the polyacrylamide material has the characteristics of high mass transfer speed, large load capacity and good regeneration capacity, however, the polyacrylamide material has shrinkage or swelling phenomenon in some solvents, so that the regeneration capacity and the mechanical stability of the polyacrylamide material are poor (Wei L, xu Z, wu Y L, et al program on hydrogels for the removal of heavy metal from water. Journal of Hubei University (Natal Science), 2017,39 (1): 30-15.Wu M,WU R,Zhang Z,et al.Preparation and application of organic-silica hybrid monolithic capillary columns. Electric field, 2011,32 (1): 105-115.). Polyaniline contains a large amount of amino groups due to its adjustable chemical structure, high stability and skeleton, and can be compounded with other materials, so that the specific surface area is effectively increased, and the adsorption sites are increased. However, polyaniline materials are complex to synthesize and difficult to control in morphology (Mansource M S, ossman M E, farag H A, et al, remote of Cd (II) ion from waste water by adsorption onto polyaniline coated on, sawdummy. Desamination, 2011,272 (1): 301-305.Gupta V K,Pathania D,Kothiyal N C,et al.Polyaniline zirconium (IV) silicophosphate nanocomposite for remediation of methylene blue dye from waste water. Journal of Molecular Liquids,2014,190:139-145.Shao D,Hou G,Li J,et al.PANI/GO as a super adsorbent for the selective adsorption of uranium (VI). Chemical Engineering Journal,2014,255; 604-612.). Therefore, development of an adsorption material which is simple in synthesis operation, low in cost and stable in structure and can realize rapid selective enrichment of PFCs in water is needed.
Disclosure of Invention
The invention aims to: aiming at the problems existing in the prior art, the invention provides a preparation method of an aminated polyacrylamide foam adsorbent, which can remarkably improve the problems of poor selective adsorption effect, low reusability, high cost and easiness in influence of coexisting substances of the existing adsorbent on perfluorinated compounds.
The invention also provides application of the aminated polyacrylamide foam adsorbent.
The technical scheme is as follows: in order to achieve the above object, the present invention provides a method for preparing an aminated polyacrylamide foam adsorbent, comprising the steps of:
(1) Preparing an acrylamide and N-N methylene bisacrylamide monomer original solution under a greenhouse, adding an ammonium persulfate solution and tetramethyl ethylenediamine, introducing into a mold after rotation, sealing the liquid level, and performing reaction shaping to obtain polyacrylamide;
(2) Immersing polyacrylamide into a hydrochloric acid solution, adding aniline, then adding ammonium persulfate solution for oxidation, and immersing overnight to obtain an aminated polyacrylamide gel material;
(3) And freeze-drying the obtained aminated polyacrylamide gel and firing to obtain the aminated polyacrylamide foam adsorbent.
Further, in the step (1), the mass fraction of the acrylamide is 10-20%, and the mass fraction of the N-N methylene bisacrylamide is 1-10%.
Further, the mass fraction of the ammonium persulfate solution in the step (1) is 10-20%, the adding amount is 5-10 mu L/ml of the reaction solution, and the adding amount of the tetramethyl ethylenediamine is 0.5-2 mu L/ml of the reaction solution.
Preferably, the ammonium persulfate solution in the step (1) is added in an amount of 5. Mu.L per ml of the reaction solution and tetramethyl ethylenediamine is added in an amount of 0.5. Mu.L per ml of the reaction solution.
Wherein, in the step (2), water or an organic solvent is used for sealing the liquid level, and the organic solvent is any one of isoamyl alcohol, water saturated isobutanol and acetone.
Further, the mass ratio of the acrylamide to the aniline is 1-5:1-5.
Preferably, the mass ratio of acrylamide to aniline is 1:1.
Further, the firing in step (3) uses a tube furnace firing to sinter the material in N 2 Firing for 2-4 h at 300-400 ℃ under atmosphere.
Preferably, in step (3), the material is treated in N 2 Firing for 2h at 300 ℃ under atmosphere.
The invention also provides application of the aminated polyacrylamide foam adsorbent in removing trace perfluorinated compounds in water.
Further, the application process is as follows: and (3) placing the aminated polyacrylamide foam adsorbent and the aqueous solution containing the perfluorinated compounds into a glass bottle, and placing the glass bottle into a constant-temperature oscillator for adsorption balance.
Wherein the adding amount of the aminated polyacrylamide foam adsorbent is 1-5 g/L, and the concentration of the perfluorinated compound is 1-5 mug/L.
Preferably, the aminated polyacrylamide foam adsorbent is added in an amount of 1g/L and the concentration of the perfluorinated compound is 1. Mu.g/L.
Wherein the adsorption temperature is 25+/-1 ℃ and the adsorption equilibrium time is 1-2 h.
Preferably, the adsorption temperature is 25℃and the adsorption equilibrium time is 1h.
The invention obtains Polyacrylamide (PAM) through the polymerization reaction of Acrylamide (AM) and N-N Methylene Bisacrylamide (MBA), then changes the molecular structure of the polymer through composite Polyaniline (PANI), enhances the adsorption effect and the material stability, and enhances the adsorption effect and the material stability through the polymerization reaction of the Acrylamide (AM) and N-N Methylene Bisacrylamide (MBA) 2 Heating in atmosphere to change the functional groups on the surface of the material, improve the water absorbability of the material, fully utilize pore channels and finally synthesize the aminated polyacrylamide foam composite material capable of efficiently and selectively adsorbing PFCs.
Compared with the prior art, the invention has the following remarkable advantages:
(1) The aminated polyacrylamide foam adsorbent for treating trace perfluorinated compounds in water, which is prepared by the invention, is prepared into polyaniline through polymerization reaction of aniline, is aminated and compounded on polyacrylamide foam under the oxidation of ammonium persulfate, and is prepared into a product with the following formula of N 2 Heating under atmosphere to change the functional groups on the surface of the material, improve the water absorption of the material, fully utilize pore channels, ensure that the composite foam material has a porous structure and higher specific surface area, and can increase the electrostatic adsorption effect on perfluorinated compounds by surface aminated groups.
(2) The aminated polyacrylamide foam adsorbent prepared by the invention can reach adsorption equilibrium within 15min by electrostatic adsorption and hydrophobic action and the formation of micelle inside the adsorbent and hemi-micelle on the surface of the adsorbent, the adsorption rate can reach 99.5%, the efficient selective adsorption removal of trace perfluorinated compounds in water is realized, and even the perfluorinated compounds in water are not greatly influenced by the presence of small molecular acids, salts and organic matters.
(3) The aminated polyacrylamide foam adsorbent prepared by the invention can effectively remove perfluorinated compounds in water in the pH range of 2-10, has a wide adsorption pH value, can still keep a good adsorption effect under the influence of various environmental factors, and has a good application prospect.
(4) The aminated polyacrylamide foam adsorbent provided by the invention solves the defects of weak adsorption force of activated carbon on perfluorinated compounds, extremely long adsorption equilibrium time of ion exchange resin and poor selectivity and recycling property in the traditional adsorption material, and is simple to synthesize, green, economic, nontoxic and harmless.
Drawings
FIG. 1 is a schematic diagram of the process of synthesizing an aminated polyacrylamide foam adsorbent according to the present invention;
FIG. 2 is a schematic diagram of the mechanism of the aminated polyacrylamide foam adsorbent of the present invention for adsorbing perfluorinated compounds;
FIG. 3 is a graph showing the adsorption kinetics of the aminated polyacrylamide foam adsorbent of the present invention and the polyacrylamide, unfired aminated polyacrylamide, of the control group against perfluorinated compounds in water;
FIG. 4 is a scanning electron microscope image of a polyacrylamide and aminated polyacrylamide foam adsorbent, respectively, wherein 4a is polyacrylamide and 4b is aminated polyacrylamide foam adsorbent;
FIG. 5 is an automatic mercury porosimeter average pore size distribution plot of the aminated polyacrylamide foam adsorbent of the present invention, as well as a control group polyacrylamide, unfired aminated polyacrylamide;
FIG. 6 is a graph showing the adsorption kinetics of the aminated polyacrylamide foam adsorbent of the present invention against perfluorinated compounds in water under the influence of small molecule acids;
FIG. 7 is a graph showing the adsorption kinetics of the aminated polyacrylamide foam adsorbent of the present invention against perfluorinated compounds in water under the influence of natural organic matter and salts;
FIG. 8 is a graph of the reusability of the aminated polyacrylamide foam adsorbent of the present invention for adsorbing perfluorinated compounds in water;
FIG. 9 is a graph showing the effect of the aminated polyacrylamide foam adsorbent of the present invention on the adsorption rate of perfluoro compounds in solutions of different pH values.
Detailed Description
The invention is further described below with reference to the drawings and examples.
The experimental methods described in the examples, unless otherwise specified, are all conventional. The medicines and the reagents are all conventional medicines unless specified.
Example 1
The preparation method of the aminated polyacrylamide foam adsorbent is shown in fig. 1, and comprises the following specific steps:
(1) Preparing an acrylamide and N-N methylene bisacrylamide monomer original solution under a greenhouse, and dissolving 3g of acrylamide and 0.3g of cross-linking agent N-N methylene bisacrylamide in 30mL of deionized water; degassing for 15min under a nitrogen atmosphere, and adding 150uL of ammonium persulfate solution with the mass fraction of 10% and 15uL of tetramethyl ethylenediamine into the reaction solution. The solution was rotated 10 times, and the solution was introduced into a mold without introducing air, and the solution was sealed with 1mL water to obtain polyacrylamide after reaction setting.
(2) And (3) after the polymerization reaction in the step (1) is completed, immersing the solidified polyacrylamide into a 1mol/L hydrochloric acid solution, adding aniline according to the mass ratio of the acrylamide to the aniline of 1:1, adding 300uL of oxidant 10% ammonium persulfate solution for oxidation, and immersing overnight to obtain the aminated polyacrylamide gel material.
(3) At N 2 And (3) in the atmosphere, freeze-drying the aminated polyacrylamide gel, and then firing the aminated polyacrylamide gel in a tube furnace at 300 ℃ for 2 hours to obtain the aminated polyacrylamide foam adsorbent.
The application of the aminated polyacrylamide foam adsorbent is that the aminated polyacrylamide foam adsorbent and the perfluorinated compound solution are placed in a glass bottle, so that the concentration of the aminated polyacrylamide foam adsorbent is 1g/L, the perfluorinated compound is 1 mug/L, the glass bottle is placed in a constant-temperature oscillator, the reaction rotating speed is set to 150r/min, the experimental temperature is 25+/-1 ℃, and the adsorption balance is 1h.
The aminated polyacrylamide foam adsorbent prepared by the invention realizes rapid selective adsorption enrichment of trace perfluorinated compounds in water. As shown in fig. 2, the synthesized aminated polyacrylamide foam adsorbent has a porous structure and a high specific surface area, and the surface aminated groups can increase the electrostatic adsorption effect on perfluorinated compounds, the action mechanisms of the aminated polyacrylamide foam adsorbent on perfluorinated compounds comprise electrostatic adsorption, hydrophobic effect and formation of micelles and semi-micelles on the surface of the adsorbent in the adsorbent, and the aminated polyacrylamide foam adsorbent is simple in material synthesis, low in cost, better in adsorption effect than the traditional adsorption material, good in reusability and free of secondary pollution.
Example 2
The present example mainly examined the adsorption equilibrium time and adsorption rate of the synthesized aminated polyacrylamide foam adsorbent and the control group (polyacrylamide, aminated polyacrylamide gel) to perfluorooctanoic acid (PFOA) in water, and the specific steps are as follows:
the aminated polyacrylamide foam adsorbent, polyacrylamide and aminated polyacrylamide gel prepared in example 1 with a final concentration of 1g/L are respectively added into a 20mL glass bottle with a cover; and PFOA solution with final concentration of 1. Mu.g/L, pH value of each reaction solution was adjusted to 6.+ -. 0.1 by using 1M NaOH/HCl, and the flask was placed in a constant temperature shaker, setting reaction speed of 150r/min, and experimental temperature of 25.+ -. 1 ℃.
The aminated polyacrylamide foam adsorbent and the control group (polyacrylamide, aminated polyacrylamide gel) were sampled for 1mL at 0, 1,2, 3,4, 7, 15, 30, 40, 60min at the beginning of the experiment, the PFOA content in the water sample was measured by LC-MS/MS, and the PFOA remaining ratio in the solution was calculated by the following formula (1).
As can be seen from FIG. 3, compared with the control group (polyacrylamide and aminated polyacrylamide gel), the synthesized aminated polyacrylamide foam adsorbent can reach adsorption equilibrium for PFOA with the concentration of 1 mug/L in water within 15min, the effect is obviously superior to that of the control group, the adsorption rate is 99.5%, and the removal effect meets the requirement of United states EPA.
Example 3
The embodiment mainly examines the change of the surface morphology and microstructure before and after the polyacrylamide is compounded with polyaniline to obtain the aminated polyacrylamide foam adsorbent. The method comprises the following specific steps:
the polyacrylamide and aminated polyacrylamide foam adsorbent obtained in example 1 was cut into thin sheets and then observed on a Scanning Electron Microscope (SEM) QUANTA FEG 250.
As shown in fig. 4a and 4b, the polyaniline chains after being compounded construct pore channels on the surface of the material, so that the material structure and the specific surface area can be effectively stabilized, and the adsorption effect can be enhanced.
Example 4
This example mainly examined the surface pore size of aminated polyacrylamide foam adsorbent, blank polyacrylamide, and unfired aminated polyacrylamide of control group. The method comprises the following specific steps:
2-3 g of the aminated polyacrylamide foam adsorbent obtained in example 1 and a control group (polyacrylamide, aminated polyacrylamide gel) were each taken, and the average pore diameter of the sample was measured using an Autopore IV 9510 automatic mercury porosimeter.
As can be seen from FIG. 5, the aminated polyacrylamide foam adsorbent has a richer pore size, the average pore size maximum value is about 61 μm, the amination process increases the porosity of the material and the firing process decreases the pore size of the material, so that the material has a higher specific surface area and a higher adsorption potential.
Example 5
This example mainly examined the effect of aminated polyacrylamide foam adsorbents on the adsorption equilibration time and adsorption rate of PFOA in water in the presence of small molecule acids. The method comprises the following specific steps:
into a 20mL glass bottle with a cap were added an aminated polyacrylamide foam adsorbent prepared in example 1 at a final concentration of 1g/L and an aqueous PFOA solution at a final concentration of 1. Mu.g/L, and oxalic acid (H) 2 C 2 O 4 ) Or formic acid (HCOOH) to a concentration of 5mg/L and 10mg/L, adjusting the pH value of each reaction solution to 6+ -0.1 by using 1M NaOH/HCl, placing the glass bottle in a constant temperature shaker, setting the reaction speed of 150r/min, and the experimental temperature of 25+ -1 ℃.
Sampling for 1mL at 0, 1,2, 3,4, 7, 15, 30, 40 and 60min at the beginning of the experiment, measuring the PFOA content in the water sample by using LC-MS/MS, calculating the residual ratio of PFOA in the solution by using the formula (1),comparing at H respectively 2 C 2 O 4 (5 mg/L,10 mg/L) and HCOOH (5 mg/L,10 mg/L) adsorption kinetics of PFOA in water.
As can be seen from FIG. 6, H 2 C 2 O 4 And the presence of HCOOH slightly slows down the adsorption rate of the material to PFOA, the equilibrium time is prolonged to about 30min, but the adsorption percentage is not changed greatly, so that the effect of small molecular acid on the aminated polyacrylamide foam adsorbent is not great.
Example 6
The influence of the aminated polyacrylamide foam adsorbent on the adsorption equilibrium time and the adsorption rate of PFOA in water in the presence of salts and organic matters is mainly examined in the embodiment. The method comprises the following specific steps:
the aminated polyacrylamide foam adsorbent prepared in example 1 was added to a 20mL glass bottle with a cap at a final concentration of 1g/L, and PFOA aqueous solution at a final concentration of 1. Mu.g/L, naCl was added to the glass bottle to a concentration of 5mM and 10mM, and Natural Organic Matter (NOM) was added to a concentration of 1mg/L and 5mg/L, pH values of the respective reaction solutions were adjusted to 6.+ -. 0.1 using 1M NaOH/HCl, and the glass bottle was placed in a constant temperature shaker at a reaction speed of 150r/min and an experimental temperature of 25.+ -. 1 ℃.
Samples were taken at 0, 1,2, 3,4, 7, 15, 30, 40, 60min at the beginning of the experiment for 1mL, PFOA content in the water sample was measured by LC-MS/MS, the PFOA content in the solution was calculated, and the adsorption kinetics of the material on PFOA in water in the presence of NaCl (5 mM,10 mM) and NOM (1 mg/L,5 mg/L), respectively, were compared.
As can be seen from FIG. 7, the presence of NaCl and NOM slightly slows down the PFOA adsorption rate of the material, the equilibration time is prolonged to about 35min, and the adsorption percentage is slightly reduced under the influence of NaCl but still meets the standards required by the United states environmental protection agency, so that the influence of salts and natural organic matter aminated polyacrylamide foam adsorbents is not great.
Example 7
This example mainly examined the recycling effect of aminated polyacrylamide foam adsorbents. The method comprises the following specific steps:
the aminated polyacrylamide foam adsorbent prepared in example 1 with a final concentration of 1g/L and PFOA solution with a final concentration of 1. Mu.g/L were added to a 20mL glass bottle with a cover, the pH value of each reaction solution was adjusted to 6.+ -. 0.1 using 1M NaOH/HCl, the glass bottle was placed in a constant temperature shaker, the reaction speed was set to 150r/min, the experimental temperature was 25.+ -. 1 ℃ and 1mL was sampled after 1h, and the PFOA content in the water sample was measured by LC-MS/MS.
The aminated polyacrylamide foam material after reaction is placed in 5mL of methanol (MeOH), and is oscillated for 10 hours in a constant temperature oscillator at a rotation speed of 150r/min, the aminated polyacrylamide after desorption is taken out, washed, dried and re-adsorbed to the concentration of 1 mug/L PFOA, and the desorption process is repeated for 5 times.
As shown in FIG. 8, after 5 times of recycling, the removal rate of the aminated polyacrylamide foam adsorbent to 1 mug/L PFOA is still over 92 percent, and the aminated polyacrylamide foam adsorbent has good recycling property.
Example 8
This example mainly examined the effect of aminated polyacrylamide foam adsorbents in solutions of different pH values on the adsorption rate of PFOA. The method comprises the following specific steps:
the aminated polyacrylamide foam adsorbent prepared in example 1 with a final concentration of 1g/L and PFOA solution with a final concentration of 1. Mu.g/L are added into a 20mL glass bottle with a cover, the pH values of the reaction solutions are respectively adjusted to 2, 4, 6, 8 and 10 by using 1M NaOH/HCl, the glass bottle is placed in a constant temperature oscillator, the reaction rotating speed is set to 150r/min, the experimental temperature is 25+/-1 ℃, 1mL is sampled after 1h, and the PFOA content in the water sample is measured by using LC-MS/MS.
As can be seen from fig. 9, the aminated polyacrylamide foam adsorbent has a good PFOA removal effect at a wide range of pH.
Claims (10)
1. The preparation method of the aminated polyacrylamide foam adsorbent is characterized by comprising the following steps of:
(1) Preparing an acrylamide and N-N methylene bisacrylamide monomer original solution, adding an ammonium persulfate solution and tetramethyl ethylenediamine, rotating, introducing into a mold, sealing the liquid level, and performing reaction and shaping to obtain polyacrylamide;
(2) Immersing polyacrylamide into a hydrochloric acid solution, adding aniline, then adding an ammonium persulfate solution, and immersing overnight to obtain an aminated polyacrylamide gel material;
(3) And freeze-drying the obtained aminated polyacrylamide gel and firing to obtain the aminated polyacrylamide foam adsorbent.
2. The method for preparing the aminated polyacrylamide foam adsorbent according to claim 1, wherein the mass fraction of the acrylamide in the step (1) is 10-20%, and the mass fraction of the N-N methylene bisacrylamide is 1-10%.
3. The method for preparing the aminated polyacrylamide foam adsorbent according to claim 1, wherein the liquid level is sealed in the step (1) by water or an organic solvent, wherein the organic solvent is any one of isoamyl alcohol, water saturated isobutanol and acetone.
4. The method for preparing an aminated polyacrylamide foam adsorbent according to claim 1, wherein the mass fraction of the ammonium persulfate solution in the step (1) is 10 to 20%, the amount of the ammonium persulfate solution added is 5 to 10. Mu.L/ml of the reaction solution, and the amount of the tetramethyl ethylenediamine added is 0.5 to 2. Mu.L/ml of the reaction solution.
5. The method for preparing the aminated polyacrylamide foam adsorbent according to claim 1, wherein aniline is added in the step (2) according to the mass ratio of acrylamide to aniline of 1-5:1-5.
6. The method for preparing an aminated polyacrylamide foam adsorbent according to claim 1, wherein the firing in step (3) uses a tube furnace firing to fire the material under N 2 Firing for 2-4 h at 300-400 ℃ under atmosphere.
7. Use of the aminated polyacrylamide foam adsorbent prepared by the preparation method of claim 1 for removing trace amounts of perfluorinated compounds in water.
8. The application according to claim 7, wherein the process of the application is: and (3) placing the aminated polyacrylamide foam adsorbent and the aqueous solution containing the perfluorinated compounds into a glass bottle, and placing the glass bottle into a constant-temperature oscillator for adsorption balance.
9. The use of the aminated polyacrylamide foam adsorbent according to claim 8 for removing trace amounts of perfluorinated compounds in water, wherein the addition amount of the aminated polyacrylamide foam adsorbent is 1-5 g/L, and the perfluorinated compound concentration is 1-5 μg/L.
10. The use of the aminated polyacrylamide foam adsorbent according to claim 8 for removing trace amounts of perfluorinated compounds in water, wherein the adsorption temperature is 25±1 ℃, and the adsorption equilibrium time is 1 to 2 hours.
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