CN104907057B - Spinning immobilized carbonyl iron material and application thereof in water treatment - Google Patents
Spinning immobilized carbonyl iron material and application thereof in water treatment Download PDFInfo
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- CN104907057B CN104907057B CN201510303414.6A CN201510303414A CN104907057B CN 104907057 B CN104907057 B CN 104907057B CN 201510303414 A CN201510303414 A CN 201510303414A CN 104907057 B CN104907057 B CN 104907057B
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Abstract
The invention discloses a spinning immobilized cage-like carbonyl iron nano particle and application of the spinning immobilized cage-like carbonyl iron nano particle. The electrostatic spinning technology is adopted to immobilize a cage-like carbonyl iron material to prepare the spinning immobilized carbonyl iron material, and dissolved heavy metal ions in water are removed in an adsorption mode. The prepared adsorbing agent has high adsorption rate, the concentrations of heavy metal antimony and selenium are reduced to be lower than the limit value of the concentrations of drinking water when the adsorbing agent is added, more than 95% of heavy metal antimony and selenium are removed within 100min, and 97% of arsenic can be removed within 150min. The adsorption rate of the adsorption material is considerably higher than that of the other composite adsorbing materials, and the adsorbing effect of the adsorbing agent is stable; compared with other treatment modes, the method can shorten the reaction time and the treatment expenses; the spinning immobilized cage-like carbonyl iron nano particle has excellent separation property, water body after adsorption treatment is not required to be filtered and separated, and the heavy metal adsorption removal technology is particularly suitable for large-scale industrialized application.
Description
Technical field：
The invention belongs to heavy metal in water ion remaval technical field, more particularly to one kind are fixed by electrostatic spinning technique
Caged hydroxyl iron material and its high toxicity heavy metal common to water body removal.
Background technology：
In recent years, the developing rapidly industrially with China, the environmental problem for increasingly increasing also is subject to increasing
Pay attention to.In particular with high concentration, high toxicity heavy metal is due to discharge beyond standards and is not good at disposing, in surface water and subsoil water
Accumulation, seriously threaten the health and safety of the mankind.Arsenic, antimony, selenium are opened as heavy metal common in polluted-water in mine
Adopt, be widely present in the trade effluent of pigment and dyestuff processing and other fields, cause content of beary metal severe overweight in industrial water drainage,
Have a strong impact on the water quality and the safety of neighbouring drinking water source of peripheral ground water and subsoil water.In addition, some regional drinking water sources
Heavy Metals in Waters content there is also exceeded phenomenon.It is how cost-effective to remove the heavy metal retained in water body, reduce work
Threat of the industry draining to ecological environment has become current water environment field problem demanding prompt solution.
At this stage, mainly there are the sedimentation method, oxidation-reduction method, ion exchange, life to the minimizing technology of heavy metal in environment
Thing method and absorption method etc..From the point of view of considering, absorption method is cheap, efficiently, it is stable the characteristics of, applicable elements extensively, operation
The advantage such as simple, it has also become the prefered method of industrial heavy metal in water purification.But in actual applications it was found that conventional inhale
Attached dose has that adsorption capacity is little, absorption stability is poor, adsorption time length, treatment effect are vulnerable to ambient conditions such as pH, temperature with
And the impact of coexisting ion etc., and need to carry out after-treatment to water body after absorption after adsorbent is added, increased water body net
Change the operation for processing.Based on problem above, the good adsorbing material of new, easily separated and adsorption effect becomes urgently to be developed
Emphasis.
Electrostatic spinning technique be it is at present general solution or melt substance are changed into continuously, diameter arrive several at several microns
The material preparation technology of the continuous rope between nanometer.The operational approach of electrostatic spinning technique is simple, preparation cost is cheap,
And obtained spinning film have the advantages that larger specific surface area, it is stable in properties, be easily isolated recovery.Meanwhile, the technology can be with
The functional particles with different shape such as inorganic salt are combined on polymer fiber, and in composite with higher concentration
Preparation field has broad application prospects.The composite cellulosic membrane adsorbing material constantly developed based on electrostatic spinning technique,
Good absorption property is shown to heavy metal pollutants in water, to common heavy metal polluter Cu2+、Cd2+、As5+Deng
Adsorption capacity can respectively reach 161.29mg/g, 357.14mg/g (Wang X.F., et al., Poly
(ethyleneimine)nanofibrous affinity membrane fabricated via one step wet-
electrospinning from poly(vinyl alcohol)-doped poly(ethylenemine)solution
system and its application[J].Journal of Membranes Science,2011,397,191-120)
7.1mg/g(Min L L.,et al.,Preparation of a novel iron oxide/chitosan composite
nanofiber and its adsorption of arsenate from water[J].Acta Scientiae
Circumstantiae,2014,34(12),2979-2984).From suction of the existing composite fiber membrane material to heavy metal in water
From the point of view of attached effect, electrostatic spinning nano fiber film can effectively be removed with heavy metal polluter really, but removal rate
Have much room for improvement with adsorption capacity.This requires to select the adsorbing material with higher adsorption activity more to be had with spinning fibre
The combination of effect, is also the research emphasis for preparing easily separated adsorption cleaning material.
Traditional adsorbing material --- iron carbonyl, it is industrially wide because of its good absorption property and property cheap and easy to get
General application.But the close structure of traditional iron carbonyl can serious limit pollution thing to its internal migration, reduce adsorbate and its surface
The contact of avtive spot.From the point of view of structure angle, the adsorbing material of lamellar structure not only can be by the adsorption activity on its surface
Site effectively discharges, and can largely increase the specific surface area of material so that adsorbate and suction in solution
The avtive spot on attached dose of surface is fully contacted, and improves its absorption property.Therefore, a kind of employing is etched prepared by template by us
Caged hydroxyl iron material is incorporated in the preparation of spinning fibre film, and the avtive spot for making full use of this hydroxyl iron material abundant is carried
Adsorption capacity of the high spinning fibrous membrane in heavy metal adsorption, to realize that spinning membrane material heavy metal is rapid, efficiently remove.
In sum, this fiber film material by caged hydroxyl iron material in combination with electrostatic spinning is with caged material
The double dominant of material and membrane material：The hydroxyl that iron carbonyl material surface not only can be caused is fully used, largely
The active adsorption sites of material surface are increased, can guarantee that the composite has excellent separating property again, it is to avoid after absorption
The after-treatment of water body.This composite fiber membrane material obtains good adsorption effect in heavy metal in water adsorption cleaning field,
Largely solve to be difficult to detached problem to heavy metal in water purification removal and adsorbent in engineering and commercial Application.
The content of the invention
In order to solve the above problems, the present invention is using the side that caged hydroxyl iron nano-particle is fixed on spinning fibre film
The good adsorbing material of method preparative separation function admirable, absorption property, and depth is carried out to arsenic, antimony, three kinds of heavy metal in water of selenium
Purification is removed, and makes every effort to be reduced to industrial water drainage with the concentration of these three heavy metals in drinking water resource《Drinking Water quality
Standard》(GB5749-2006) in below the concentration of defined, to solve arsenic, antimony, selenium these three heavy metal substances to surrounding
And the potential threat that health is present.Reduce processing cost and intractability, avoid adsorb after water body after-treatment it is same
When ensure adsorption treatment after water outlet reach water quality standard for drinking water.
For achieving the above object, the present invention proposes the side being fixed to caged hydroxyl iron nano-particle on spinning fibre film
Method, body step is as follows：
(1) preparation of caged iron carbonyl：
First 3.8g polyvinylpyrrolidones are dissolved in into 50mL concentration for 0.1mol/L in the presence of magnetic stirring apparatuss
In dilute hydrochloric acid, it is to be dissolved completely after, 110mg potassium ferrocyanides are added in above-mentioned mixed liquor, stir to forming settled solution.
The settled solution is transferred in 80 DEG C of constant temperature ovens again reacts 24h, blue deposit is can be observed and generates.After isothermal reaction
The deposit of gained is transferred in centrifuge tube, and supernatant is outwelled after centrifugation, is obtained pure blue deposit and is pure ferrous iron
Ferricyanide.
Ultra-pure water is added in the blue deposit of above-mentioned gained, and deposit is fully dispersed under ultrasound condition
In ultra-pure water.Again Jing after supernatant is removed in centrifugation, dehydrated alcohol, Jing ultrasounds is added to make deposit breakup in ethanol in deposit
Afterwards recentrifuge removes supernatant.
Add dehydrated alcohol, ultrasound to be completely dispersed it in most backward blueness deposit, then be with 50mL concentration by it
The sodium hydroxide solution mixing of 0.2mol/L.This mixed solution is placed on rotary shaker after hybrid reaction 12h, gained is prepared
Blue ferric ferrocyanide deposit be gradually transformed into crocus, the precipitation obtained by Jing centrifugations is caged iron carbonyl nanometer
Grain.
(2) electrostatic spinning technique fixes the preparation of caged iron carbonyl：
Polyacrylonitrile is added in DMF first, in the presence of magnetic agitation it is completely dissolved,
Obtain precursor liquid；Subsequently by caged hydroxyl iron nano-particle Jing centrifugations post-drying obtained in step (1), moisture removal is thoroughly removed；Will
Dry caged hydroxyl iron material is added in above-mentioned precursor liquid, and its mix homogeneously is made in the presence of magnetic agitation, is contained
There is the spinning liquid of caged iron carbonyl.Finally spinning liquid is injected in the syringe with draw point, and is connected with high-pressure spinning machine.
The filament for obtaining is sprayed via high-pressure spinning machine and is the spinning material for combining caged iron carbonyl, namely final required Jing
Electrostatic spinning immobilized caged hydroxyl iron material.
The polyacrylonitrile consumption is 0.7-1g；
The N,N-dimethylformamide consumption is 5-15mL；
Cage-like iron carbonyl dosage is 0.05-0.1mg；
Beneficial effect：
1) present invention is first fixed caged hydroxyl iron material using the technology of electrostatic spinning, is prepared spinning and is fixed
Change hydroxyl iron material.The heavy metal ion of the dissolved in eliminating water is gone by way of absorption.
2) adsorbing material prepared by the present invention has higher adsorption capacity and the faster rate of adsorption, can be in 100min
It is interior that heavy metal antimony, selenium are removed into more than 95%, arsenic is removed into 97% in 150min.The adsorption capacity of the adsorbing material is far above
Other composite adsorbing materials, and treatment effect is stable；Compared with other processing modes, response time and processing cost are reduced.
3) adsorbing material prepared by the present invention is in film like, can directly from taking-up in water body is processed be had after use
Excellent separating property, it is to avoid dispersed adsorbing material is separated by filtration in water body after processing so that Adsorption heavy metal
Technology be more suitable for industrialization large-scale application.
Description of the drawings
Fig. 1 caged iron carbonyls prepare the electron microscopic picture of predecessor ferric ferrocyanide；
The electron microscopic picture of Fig. 2 caged iron carbonyls；
The transmission electron microscope picture of Fig. 3 caged iron carbonyls；
Fig. 4 is fixed on the caged iron carbonyl electron microscopic picture on electrostatic spinning；
Adsorption effect of the immobilized caged iron carbonyls of Fig. 5 to heavy metal in water
Wherein, (a) be pentavalent arsenic, (b) be trivalent antimony, (c) be tetravalence selenium；
Wherein, solid line is that Freundlich Adsorption Models dotted line is Langmuir Adsorption Models；
The immobilized caged iron carbonyl heavy metals of Fig. 6 pollute the treatment effect of actual water body
Wherein, (a) be trivalent arsenic+pentavalent arsenic, (b) be trivalent antimony, (c) be tetravalence selenium
Specific embodiment
Embodiment 1：A kind of preparation method of caged iron carbonyl
1st, the preparation of caged iron carbonyl：
At ambient temperature, 3.8g PVP K-30s are dissolved in the presence of magnetic stirring apparatuss first
In 50mL 0.1mol/L dilute hydrochloric acid, it is to be dissolved completely after, 110mg potassium ferrocyanides are added in above-mentioned mixed liquor, continue to stir
30min is mixed, until forming settled solution.The settled solution is transferred in 80 DEG C of constant temperature ovens again reacts 24h, it can be observed that
Blue deposit is generated.The deposit of gained after isothermal reaction is transferred in centrifuge tube, is centrifuged after 15min under 7500rpm
Supernatant is outwelled, pure blue deposit is obtained.Ultra-pure water is added in the blue deposit of above-mentioned gained, and causes deposit
It is fully dispersed in ultra-pure water in the case where ultrasound is adjusted.It is centrifuged under the conditions of 7500rpm again after 15min and outwells supernatant, then to
Dehydrated alcohol is added in deposit, Jing after ultrasound makes deposit breakup in ethanol, again 15min is centrifuged under 7500rpm.Finally
Supernatant is removed, the blue deposit of gained is pure ferric ferrocyanide.10ml is added in the blue deposit of gained
Dehydrated alcohol, ultrasound is completely dispersed it, then it is mixed with 50mL 0.2mol/L sodium hydroxide.This mixed solution is put
Mix after 12h on rotary shaker, the blue ferric ferrocyanide deposit obtained by preparation is gradually transformed into crocus, then Jing
Caged hydroxyl iron nano-particle is just obtained after 7500rpm centrifugation 15min.
Fig. 1 is the electron microscopic picture of the predecessor ferric ferrocyanide of caged iron carbonyl prepared by embodiment 1, can be with bright from figure
It is aobvious to observe that the ferric ferrocyanide obtained by preparing has well-regulated cubic shaped, arrange loose, and size is homogeneous, disperses journey
Degree is preferable.
Fig. 2 is the electron microscopic picture of caged hydroxyl iron nano-particle prepared by embodiment 1, it can be seen that the etching of sodium hydroxide
The cubic morphology of material is not destroyed, and the surface of otherwise smooth becomes loose, is conducive to and the pollutant in water body
Matter is contacted.
Fig. 3 is the transmission electron microscope picture of caged iron carbonyl prepared by embodiment 1, it can be observed that the material is in microcosmic point
On present loose hollow structure, be further characterized by what caged iron carbonyl was made up of five lamellas being closely joined together
The cube structure of rule.
Embodiment 2：A kind of electrostatic spinning fixes the preparation method of caged iron carbonyl
Caged hydroxyl iron material obtained by preparing in embodiment 1 first high speed centrifugation 2min under 10000rpm so as to
Middle remaining moisture is thoroughly removed；Secondly, 800mg polyacrylonitrile is added in 10mL DMFs, in magnetic force
Be completely dissolved polyacrylonitrile in the presence of stirring, mix homogeneously, as the precursor liquid of spinning liquid；Subsequently, 0.1mg Jing are centrifuged
The caged iron carbonyl for removing moisture removal mixes with above-mentioned precursor liquid, and mix homogeneously is continued under the conditions of magnetic agitation；Finally, will
Spinning liquid containing caged iron carbonyl is transferred to be furnished with the syringe of rustless steel syringe needle, and is assembled on high-pressure spinning machine.Spin
Filament voltage is set as 20KV, and solution is advanced by peristaltic pump, and fltting speed is 1mL per minute.The filament ejected is
Combine the spinning material of caged iron carbonyl.
Fig. 4 is the electron microscopic picture of the caged hydroxyl iron material being fixed on electrostatic spinning of the gained of embodiment 2, can from figure
To find out, caged hydroxyl iron material is connected in thread spinning in string-of-pearls-like, and the caged iron carbonyl that Jing spinning is combined is not
Have and change its basic configuration, the immobilization of adsorbing material can't bring greater impact to the absorption property of material.
Embodiment 3：A kind of electrostatic spinning fixes the preparation method of caged iron carbonyl
Caged hydroxyl iron material obtained by preparing in embodiment 1 first high speed centrifugation 2min under 10000rpm so as to
Middle remaining moisture is thoroughly removed；Secondly, 700mg polyacrylonitrile is added in 5mL DMFs, in magnetic force
Be completely dissolved polyacrylonitrile in the presence of stirring, mix homogeneously, as the precursor liquid of spinning liquid；Subsequently, by 0.05mg Jing from
The heart goes the caged iron carbonyl of moisture removal to mix with above-mentioned precursor liquid, and mix homogeneously is continued under the conditions of magnetic agitation；Finally,
Spinning liquid containing caged iron carbonyl is transferred to and is furnished with the syringe of rustless steel syringe needle, and be assembled on high-pressure spinning machine.
Spinning voltage is set as 20KV, and solution is advanced by peristaltic pump, and fltting speed is 1mL per minute.The filament ejected is i.e.
To combine the spinning material of caged iron carbonyl.
Embodiment 4：A kind of electrostatic spinning fixes the preparation method of caged iron carbonyl
Caged hydroxyl iron material obtained by preparing in embodiment 1 first high speed centrifugation 2min under 10000rpm so as to
Middle remaining moisture is thoroughly removed；Secondly, 1000mg polyacrylonitrile is added in 15mL DMFs, in magnetic
Power is completely dissolved polyacrylonitrile in the presence of stirring, mix homogeneously, used as the precursor liquid of spinning liquid；Subsequently, by 0.075mg Jing
Centrifugation goes the caged iron carbonyl of moisture removal to mix with above-mentioned precursor liquid, and mix homogeneously is continued under the conditions of magnetic agitation；Most
Afterwards, the spinning liquid containing caged iron carbonyl is transferred to and is furnished with the syringe of rustless steel syringe needle, and be assembled to high-pressure spinning machine
On.Spinning voltage is set as 20KV, and solution is advanced by peristaltic pump, and fltting speed is 1mL per minute.The filament ejected
As combine the spinning material of caged iron carbonyl.
Embodiment 5：Method for adsorbing and purifying of the electrostatic spinning immobilized caged hydroxyl iron material to heavy metal in water
Actual heavy metal-polluted water is simulated with the sewage containing 1mg/L low-concentration arsenics, three kinds of ions of antimony and selenium respectively, and
The immobilized caged hydroxyl iron material that embodiment 2 prepares gained is added in polluted water body, throwing amount is 0.25g/L, is used
Dilute hydrochloric acid and dilute sodium hydroxide adjust solution p H-number between 6～7.With the carrying out of reaction, inhaled with syringe in significant interval
Take a certain amount of mixed solution and remaining concentration of heavy metal ion in settled solution is determined Jing after 0.22 μm of membrane filtration, and counter push away
To the heavy metal ion amount of Adsorption.
Fig. 5 be spinning immobilization hydroxyl iron material obtained in embodiment 2 to arsenic, antimony, selenium adsorption effect.In order to determine
The spinning immobilization hydroxyl iron material of preparation to arsenic, antimony, selenium absorption property, initial concentration and molten is shown in solution in figure
Impact of the liquid original ph to absorption property.From the experimental result of different original ph can be seen that acid condition be conducive to arsenic,
The absorption of antimony, selenium.Freundlich moulds are can be seen that from the fitting result of two kinds of Adsorption Models of Freundlich and Langmuir
Type more meets the real process of absorption, illustrate iron carbonyl to arsenic, antimony, three kinds of materials of selenium absorption closer to polymolecular layer change
Learn adsorption process.Under saturation adsorption conditionses, absorption result is fitted using Langmuir curves, its fitting result shows
Show, 250mg/g can reach to the maximal absorptive capacity of As (V)；2563mg/g may be up to the saturated extent of adsorption of Sb (V)；To Se
(IV) adsorption capacity can reach 170mg/g.
Spinning immobilization hydroxyl iron materials of the Fig. 6 obtained by the preparation of embodiment 2 is to containing respectively arsenic, antimony, three kinds of huge sum of moneys of selenium
The purified treatment design sketch of the actual water body of simulation of category polluter.It can be seen that immobilized hydroxyl iron material can
With under conditions of in pH as 6～7, the concentration of arsenic, antimony, selenium is reduced to into reduced levels in 120min.This result shows, incites somebody to action
Adsorbing material is fixed on the absorption property that on electrostatic spinning can still make caged material itself good and is not fully exerted, in water body
The heavy metal for retaining can keep the rate of adsorption faster and preferable absorbability.
Contrasted with the adsorption effect of existing adsorbent, the spinning immobilization hydroxyl iron material tool obtained by present invention preparation
There are superior adsorbing heavy metal in water arsenic, antimony, the ability of selenium and good separating property.Main cause is：First, cube knot
The caged hydroxyl iron material of structure has larger specific surface area and a large amount of fully exposed surface active groups, is being lifted and absorption
Adsorption reaction can be effectively carried out while matter contact probability；Secondly, in caged hydroxyl of the spinning surface in string-of-pearls-like arrangement
Iron material can largely retain the advantage of cage structure, make adsorbing material main body as much as possible and adsorbate in solution
Haptoreaction；Finally, the characteristic that static spinning membrane is easy to be separated from the water in itself provides excellent separation for the adsorbing material
Performance, it is to avoid the problem of after-treatment is carried out to water body after absorption.
Electrostatic spinning immobilized caged hydroxyl iron material arsenic, antimony, selenium in polluted-water are had the rate of adsorption faster and
Larger adsorption capacity, and material preparation flow itself is simple, low in raw material price, can keep in water good separation property
Energy and mechanical performance, are not only that extensively application, there is provided good condition, also becomes the guiding of adsorbing material development from now on for industry.
Claims (7)
1. a kind of preparation method of spinning immobilization hydroxyl iron material, it is characterised in that comprise the following steps that：
(1) preparation of caged iron carbonyl：
First 3.8g polyvinylpyrrolidones are dissolved in into 50mL concentration in 0.1mol/L dilute hydrochloric acid, it is to be dissolved completely after, will
110mg potassium ferrocyanides are added in above-mentioned mixed liquor, are stirred to formation settled solution, then the settled solution is transferred to into 80 DEG C
24h is reacted in constant temperature oven, blue deposit is generated, the deposit centrifugation of gained after isothermal reaction is obtained into pure blue deposition
Thing is pure ferric ferrocyanide；
It is ultrasonic respectively using dehydrated alcohol is added in blue deposit again after the above-mentioned blue deposit of pure water and washing with alcohol
It is completely dispersed, then its sodium hydroxide solution with 50mL concentration for 0.2mol/L is mixed, mixed solution is placed in rotation and shakes
On bed after hybrid reaction 12h, the blue ferric ferrocyanide deposit obtained by preparation is gradually transformed into crocus, obtained by Jing centrifugations
Precipitation is caged hydroxyl iron nano-particle；
(2) electrostatic spinning technique fixes caged iron carbonyl：
Polyacrylonitrile is completely dissolved in DMF first, obtains precursor liquid；It is subsequently that step (1) is obtained
Caged hydroxyl iron nano-particle Jing is centrifuged post-drying, thoroughly removes moisture removal；Dry caged hydroxyl iron material is added to above-mentioned
In precursor liquid, mix homogeneously obtains the spinning liquid containing caged iron carbonyl；Finally spinning liquid is injected into into the injection with draw point
In device, and it is connected with high-pressure spinning machine, the filament for obtaining is sprayed via high-pressure spinning machine and as combines caged iron carbonyl
Spinning material, namely spinning immobilization hydroxyl iron material.
2. a kind of preparation method of spinning immobilization hydroxyl iron material as claimed in claim 1, it is characterised in that described poly- third
Alkene nitrile consumption is 0.7-1g.
3. a kind of preparation method of spinning immobilization hydroxyl iron material as claimed in claim 1, it is characterised in that the N, N-
Dimethylformamide consumption is 5-15mL.
4. a kind of preparation method of spinning immobilization hydroxyl iron material as claimed in claim 1, it is characterised in that cage-like
Iron carbonyl dosage is 0.05-0.1mg.
5. a kind of preparation method of spinning immobilization hydroxyl iron material as claimed in claim 1, it is characterised in that the electrostatic
Spining technology fix caged iron carbonyl the step of be：
(1) caged hydroxyl iron material high speed centrifugation 2min under 10000rpm so as to which middle remaining moisture is thoroughly removed；
(2) 800mg polyacrylonitrile is added in 10mL DMFs, poly- third is made in the presence of magnetic agitation
Alkene nitrile is completely dissolved, mix homogeneously, used as the precursor liquid of spinning liquid；
(3) go the caged iron carbonyl of moisture removal to mix with above-mentioned precursor liquid 0.1mg Jing centrifugations, under the conditions of magnetic agitation it is made
Continue mix homogeneously and obtain spinning liquid；
(4) spinning liquid containing caged iron carbonyl is transferred to and is furnished with the syringe of rustless steel syringe needle, and be assembled to high pressure spinning
Silk machine on, spinning voltage is set as 20KV, and solution is advanced by peristaltic pump, fltting speed be 1mL per minute, the silk for ejecting
Shape thing is the spinning material for combining caged iron carbonyl.
6. such as the spinning immobilization hydroxyl iron material of any one method preparation of claim 1-5.
7. application of the spinning immobilization hydroxyl iron material as claimed in claim 6 in heavy metal pollution is processed.
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| CN106000330A (en) * | 2016-07-06 | 2016-10-12 | 中国科学院生态环境研究中心 | Hollow cubic iron-aluminum composite oxyhydroxide defluorination adsorbent based on electrospining immobilization |
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