CN107151030A - A kind of preparation method and applications for polymerizeing zirconium chloride inorganic polymer coagulant - Google Patents
A kind of preparation method and applications for polymerizeing zirconium chloride inorganic polymer coagulant Download PDFInfo
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- CN107151030A CN107151030A CN201710472339.5A CN201710472339A CN107151030A CN 107151030 A CN107151030 A CN 107151030A CN 201710472339 A CN201710472339 A CN 201710472339A CN 107151030 A CN107151030 A CN 107151030A
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- zirconium chloride
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- inorganic polymer
- polymer coagulant
- polymerization
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G25/00—Compounds of zirconium
- C01G25/04—Halides
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/52—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
- C02F1/5236—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities using inorganic agents
Abstract
The invention discloses a kind of for inorganic polymer coagulant of water process and preparation method thereof.The inorganic polymer coagulant is polymerization zirconium chloride, using zirconium chloride and high alkali liquid as raw material, high alkali liquid is added slowly in zirconium chloride solution, obtain different suitable basicities, high alkali liquid is added dropwise process control and completed in 3h, 3 5h are persistently stirred afterwards, are in the liquid of water white transparency to solution.The inorganic polymer coagulant that the present invention is provided has the advantages that product stability is good, strong to the adsorption bridging ability of colloidal substance, coagulation effect is good, wide using scope, the fields such as feedwater, wastewater treatment, papermaking, textile printing and dyeing, daily-use chemical industry are widely portable to, and with good water treatment efficiency.The inventive method have technique it is simple and direct, economical, it is quick the features such as.
Description
Technical field
The present invention relates to water-treatment technology field, more particularly to a kind of polymerization zirconium chloride inorganic polymer coagulant
(PZC) preparation method and its purposes as water treatment agent.
Background technology
Iron system or Al-based coagulant are rich in the hydrolysate of a variety of high positive charges.To improve coagulation effect, often by Al and Fe
Salt obtains the products such as aluminium polychloride, poly-ferric chloride and bodied ferric sulfate by prehydrolysis.However, Al-based coagulant is a large amount of
It is remaining using a certain amount of Al can be produced, potential hazard is produced to human health；The use of ferric flocculant is same adjoint
Problem, such as Fe salt remaining in water has compared with severe corrosive after handling.Therefore the novel flocculation with high coagulation efficiency is prepared
Agent is imperative.Other alternative metal ions, such as Zr salt are being taken seriously in the application of water treatment field.It is worth referring to
Go out to be the coagulant based on Zr elements have a higher positive charge amount than Al and Fe coagulant, reachable+8 valency of highest valence state, this
Charge neutrality ability is greatly improved, and then promotes contaminant removal efficiency.On the other hand, Zr does not possess toxicity, most of
Exist under the pH level related to biological activity in inert dioxide form.Compared to traditional Al systems coagulant, Zr pairs
Human body does not result in potential injury, it ensure that sewage and the security of drinking water treatment.
But zirconium chloride solution sheet is as highly acid, zirconium chloride is used as coagulant, in hydrolytic process also due to
Hydrolysis and discharge substantial amounts of H+, the pH that these factors result in coagulation water outlet is relatively low, and this shortcoming has had a strong impact on it
The later use of water outlet and further processing.
Therefore, people are still desirable to obtain a kind of with high positive charge hydrolysate, can obtain at lower doses
High organic pollutant removal rate, has the advantages that the coagulant that coagulation efficiency is high, stability is good, harmless, applied widely.
The content of the invention
It is an object of the invention to provide a kind of preparation method for polymerizeing zirconium chloride inorganic polymer coagulant, thus obtain
Obtain a kind of green, efficient novel inorganic high-molecular coagulant adopting.
To achieve the above object, the present invention is provided as in terms of several：
<1>A kind of preparation method for polymerizeing zirconium chloride inorganic polymer coagulant, it is as follows that methods described includes step：
(1) 10%-20% (w/v) ZrCl is configured with deionized water4Solution；
(2) at 0-4 DEG C, by ZrCl4Solution is under conditions of stir speed (S.S.) is 300-800rpm lasting stirring, by concentration
ZrCl is added slowly in 80-200g/L concentrated alkali solution4In solution so that basicity in the range of more than 0 to 2.5, wherein
Basicity=[OH-]/[Zr4+],
(3) above-mentioned steps (2) concentrated alkali solution adding procedure adds time control within 3h according to the difference of basicity,
Then proceed to stir 3-5h, obtain transparent clarification and in the absence of the solution of visible precipitate thing, that is, the polymerization of different basicities is made
Zirconium chloride inorganic polymer coagulant solution.
<2>According to the preparation method of the polymerization zirconium chloride inorganic polymer coagulant of above one, wherein, in step
(1) in, use quality concentration is 98%-100% ZrCl4It is configured to described ZrCl4Solution.
<3>, according to the preparation method of the polymerization zirconium chloride inorganic polymer coagulant described in above any one, wherein,
Predetermined basicity described in step (2) is 0.2-2.5.
<4>, polymerization zirconium chloride inorganic polymer coagulant according to any one of above claim 1 preparation side
Method, wherein the concentrated alkali solution is selected from sodium hydroxide solution and potassium hydroxide solution.
<5>, according to the preparation method of the polymerization zirconium chloride inorganic polymer coagulant described in above any one, wherein,
In step (2), concentrated alkali solution is added in the way of being added dropwise to the ZrCl prepared by step (1)4In solution.
<6>, it is a kind of according to above<1>Extremely<5>The zirconium chloride inorganic polymer that method any one of is obtained
Compound.
<7>, according to above<1>Extremely<5>The polymerization zirconium chloride inorganic polymer that method any one of is obtained
Coagulant in water process as water treatment agent purposes.
<8>, purposes according to claim 7, the purposes include will be according to above<1>Extremely<5>Any one of
The polymerization zirconium chloride inorganic polymer coagulant that described method is prepared is directly appended to need water to be processed or sewage
In.
<9>, basis<7>Described purposes, wherein, the dosage of the polymerization zirconium chloride inorganic polymer coagulant is
10-40mg/ rises water or sewage, and the pH scopes of the water or waste water are 4-10.
<10>, basis<8>Described purposes, it is described need to water to be processed or sewage include feedwater, drinking water or from making
Waste water in paper, mining, textile printing and dyeing and filed of daily-use chemical industry.
Embodiment
The first aspect of the invention there is provided a kind of preparation method for polymerizeing zirconium chloride inorganic polymer coagulant,
It is as follows that methods described includes step：
(1) it is 10%-20% (w/v) (concentration for corresponding to 111.11-222.22g/L) with deionized water configuration concentration
ZrCl4Solution
(2) by ZrCl4It is placed in solution in ice-water bath, the condition persistently stirred for 300-800rpm c in stir speed (S.S.)
Under, concentration is slowly added dropwise to ZrCl for 80-200g/L high alkali liquid4Continue to stir 3-5h in solution, after completion of dropping；Its
Described in concentrated alkali solution and ZrCl4The throwing amount of solution is more than 0-2.5 than scope.
(3) difference of the process according to basicity is added dropwise in above-mentioned steps (2) high alkali liquid, and time for adding is controlled within 3h, so
Continue to stir 3-5h afterwards, obtained solution is transparent to be clarified and in the absence of visible precipitate thing, that is, the polymerization of different basicities is made
Zirconium chloride inorganic polymer coagulant solution.
Used deionized water is the deionized water on ordinary meaning in the present invention.
The raw material of the present invention is commercially available ZrCl4Powder, its mass concentration scope is 98%-100%.
In the present invention, used high alkali liquid can be sodium hydroxide, potassium hydroxide etc..It is, for example, possible to use concentration
To preferably use the NaOH or potassium hydroxide solution of the concentration that concentration is 100-180g/L.
Preferably, it is by the ZrCl of certain mass in step (1)4It is slowly added in deionized water, is transferred to volumetric flask
In, constant volume prepares 10%-20% (w/v) ZrCl4Solution.
Preferably, in step (2), described predetermined basicity is preferably 0.2-2.5, wherein basicity more than 0 to 2.5
=[OH-]/[Zr4+], for example, it is 0,0.2,0.5,1.0,1.5,2.0,2.5 that basicity, which can be basicity,.
Preferably, in step (2), ZrCl4Solution is placed in ice-water bath after 0.5-1h, starts that alkali lye, rate of addition is added dropwise
Scope can be controlled in 0.03-0.1mL/min.
Preferably, in step (2), stir speed (S.S.) is 300-800rpm.
Preferably, in step (3), high alkali liquid such as sodium hydroxide solution time for adding control is in 0.5-3h, i.e., according to institute
Predetermined basicity, adds sodium hydroxide solution within 3h.
Preferably, in step (3), after high alkali liquid such as sodium hydroxide solution completion of dropping, continue to stir 3-4h.
Second aspect of the present invention there is provided as the polymerization zirconium chloride inorganic polymer prepared by the method for the present invention
Compound.Polymerization zirconium chloride inorganic polymer coagulant (PZC) prepared by the present invention is in the absence of the colourless of visible precipitate thing
Clear solution.
The present inventor have studied the distribution of hydrolysate main signal relative intensity in ESI-TOF-MS spectrum,
As a result it is summarized in the table 1 shown in embodiment.These as shown by data, this in the present invention is made by adding concentrated alkali solution
Zirconium chloride prehydrolysis and form a kind of inorganic macromolecule compound of zirconium chloride really.As basicity value increases, greatly
Part Zr species is changed into the less high polymer of classification.Moreover, when basicity increases to 2.5, m/z values are 569 (Zr17-
Zr28) corresponding component can increase to PZC25In 26%.
In addition, polymerization zirconium chloride inorganic macromolecule compound prepared by the present invention can directly be added as coagulant
To needing in water to be processed or sewage, it is a kind of new, efficient, green water treatment agent, can be applied to feedwater, at waste water
Reason, papermaking, mining, textile printing and dyeing, filed of daily-use chemical industry.Polymerization zirconium chloride inorganic polymer coagulant is to be used for wastewater treatment
Water treatment agent, its dosage is in 10-40mg/L, and preferably dosage is 30-40mg/L, optimum dosage 40mg/L.In water
In processing, the pH scopes that polymerization zirconium chloride inorganic polymer coagulant is used are 4-10, it is preferable that pH value is 7-9.
Under in the case of being not bound by any theory, inventors believe that molten using the sodium hydroxide or potassium hydroxide of concentration
Liquid causes zirconium chloride to occur prehydrolysis and react by alkali formula titration, so can not only improve the coagulation effect of coagulant,
Also its hydrolysis in water can be slowed down to a certain extent so that its have in terms of coagulation process is controlled it is bigger excellent
Gesture.In addition, pre-hydrolysis step reduces the demand that coagulation process regulates and controls to pH, sensitivity and energy of the reduction coagulant to low temperature
It is more effective to remove pollutant.In the present invention, described " prehydrolysis " refers to control in zirconium chloride hydrolytic process by the addition of alkali
Hydrolysate.
In addition, the present inventor is also believed that the synthetic method similar to Al or Fe systems inorganic polymer, it polymerize Zr salt
There should be more preferable effect in terms of pollutant removal and reduction pH dependences than Zr salt.Preparing this kind of inorganic coagulant mistake
Cheng Zhong, metal ion there occurs in alkaline aqueous solution hydrolysis (for the hydrolysis occurred in sewage, this mistake
Journey is referred to as prehydrolysis reaction), therefore it has bigger advantage in terms of coagulation process is controlled.In addition, prehydrolysis is walked
It is rapid to reduce the demand that coagulation process regulates and controls to pH, coagulant is reduced to the sensitivity of low temperature and can more effectively remove depollution
Thing.
The polymerization zirconium chloride inorganic polymer coagulant that the present invention is obtained is compared with other coagulant with following excellent
Effect：
A) the polymerization zirconium chloride inorganic polymer coagulant for preparing of the present invention, is using zirconium chloride as raw material, using adding
Sodium hydroxide or potassium hydroxide, such as be added dropwise in the zirconium chloride solution of ice by the strong base solution of enriching by way of titration
Method be prepared from.There is high positive charge hydrolysate as coagulant, relatively low in resulting zirconium chloride solution
High organic pollutant removal rate can be obtained under dosage, with that coagulation efficiency is high, stability is good, harmless, applied widely etc. is excellent
Point.
B) present invention prepares polymerization zirconium chloride inorganic polymer coagulation using zirconium chloride as main production raw material
Agent, it is characterised in that simple production process, economy.
C) coagulant is widely portable to drinking water, wastewater treatment, and papermaking, mining, textile printing and dyeing, daily-use chemical industry etc. is led
Domain, with efficient water treatment efficiency.
Embodiment
To enable above-mentioned purpose, the feature and advantage of invention more obvious understandable, below by embodiment further more
Explain technical scheme and application effect, but these embodiments are only exemplary, and institutes of the present invention
Scope of protection is not only restricted to these embodiments.
Prepare embodiment 1
Weigh ZrCl4Powder (Wo Kai, XW100261161) 11.1111g, under 500rpm stirring conditions, is added rapidly to
In 50mL ice deionized waters, after after its dissolving, by ZrCl4Solution is transferred to 100mL volumetric flasks, and ice deionized water constant volume is obtained
10wt% ZrCl4Solution；Afterwards, 10wt% ZrCl is measured4Solution 10mL, in the case where being stirred vigorously, is dripped by alkali formula
Fixed tube is added dropwise 100g/L NaOH solution dropwise, be added dropwise volume be respectively 0.3812mL, 0.953mL, 1.906mL, 2.859mL,
3.812mL、4.765mL、5.718mL.Time for adding is respectively 10,20,40,80,120,150 minutes.Continue after completion of dropwise addition
3-5h is stirred, the inorganic height of polymerization zirconium chloride that basicity (being represented with B) is respectively 0.2,0.5,1.0,1.5,2.0,2.5 is obtained
Molecule coagulant, the product of preparation is represented with N1, N2, N3, N4, N5, N6.Using electron spray ion flight mass spectrum (ESI-TOF-
MS) Zr kinds after the hydrolysis of PZC solution that (0.2,0.5,1.0,1.5,2.0 and 2.5) synthesis is obtained under the conditions of analysis different B values
The distribution of main signal (relative intensity) see the table below 1 in class, ESI-TOF-MS spectrum.
The distribution of main signal (relative intensity) in the different basicity PZC of table 1 ESI-TOF-MS spectrum
It will be seen that with the increase of B values, most of Zr species is changed into the less high polymer of classification from table.
In B=1.5, start m/z occur in sample than high polymerization degree Zr complexs (such as Zr for 44817、Zr18、Zr19、Zr23、
Zr24、Zr26、Zr27), correspondence ratio increases to 22%.For PZC20Sample, Zr species is further hydrolyzed to the larger degree of polymerization and matched somebody with somebody
Compound, PZC20Middle m/z values reach 39% for 448 peak intensity.When basicity increases to 2.5, m/z values are 569 (Zr17-Zr28)
Corresponding component increases to PZC25In 26%.In addition, m/z values are smaller degree of polymerization species corresponding to 103 from PZC0In
51% is reduced to PZC25In 16%, m/z values be the main hydrolysate corresponding to 122 from PZC0In 71% be reduced to PZC25
In 45%.
Prepare embodiment 2
Weigh ZrCl4Powder (Wo Kai, XW100261161) 5.5556g, under 500rpm stirring conditions, is added rapidly to
In 25mL ice deionized waters, after after its dissolving, by ZrCl4Solution is transferred to 50mL volumetric flasks, and ice deionized water constant volume is obtained
10wt% ZrCl4Solution；Afterwards, 10wt% ZrCl is measured4Solution 5mL, in the case where being stirred vigorously, is dripped by alkali formula
Fixed tube is added dropwise 100g/L KOH solution dropwise, be added dropwise volume be respectively 0.2669mL, 0.667mL, 1.334mL, 2.002mL,
2.669mL、3.336mL、4.003mL.Time for adding is respectively 10,20,40,80,120,150 minutes.Continue after completion of dropwise addition
3-5h is stirred, the inorganic height of polymerization zirconium chloride that basicity (being represented with B) is respectively 0.2,0.5,1.0,1.5,2.0,2.5 is obtained
Molecule coagulant, the product of preparation is represented with N1, N2, N3, N4, N5, N6.
The inorganic polymer polymerization coagulant that the present invention is provided uses ZrCl4As raw material, sewage is handled, had
There are the performances such as higher organic pollutant removal rate.For the sake of becoming apparent from, carried out specifically below by following Application Example
The inorganic polymer polymerization coagulant that the bright present invention is provided has preferable wastewater treatment efficiency.
Application Example 1
N1, N2, N3, N4, N5, N6 polymerization zirconium chloride inorganic polymer coagulant prepared by above example 1 is used for
The processing of Kaolin clay suspension, dosage is 10-40mg/L.
Water sample preparation method：A certain amount of kaolin powder is weighed, adds in deionized water and prepares 0.25% kaolin
Suspension.Coagulation effect is represented with turbidity removal rate, while being contrasted with zirconium chloride (B=0), is represented with N0.Result
It is listed in such as table 2 below.
The polymerization zirconium chloride inorganic polymer coagulant of the different B values of table 2 is to the treatment effect of Kaolin clay suspension (with turbid
Degree clearance is represented)
From result above, turbidity removal rate lasting increase with the increase of PZC dosages, coagulation process can reach
99% kaolin clearance.These results show that these clay particles can also be assembled under low zirconium amount.When alkalization angle value
During less than 2.0, when dosage is 40mg/L, the clearance of turbidity and basicity for 0 when it is suitable, be all higher than 95%, but basicity
When increasing to 2.5, the clearance of turbidity drops to 69.4%.
Application example 2
N0 (B=0), N3 (B=1.0), N4 (B=1.5) the polymerization inorganic high scores of zirconium chloride prepared by above example 1
Sub- coagulant is used for the processing of sewage disposal plant effluent, and research polymerize the mixed of zirconium chloride under the conditions of different coagulants dosage
Solidifying effect, dosage is 15-40mg/L.Coagulation effect represents that result is listed in such as table 3 below with total organic Carbon removal.
The polymerization zirconium chloride inorganic polymer coagulant of the different B values of table 3 to the treatment effect of sewage disposal plant effluent (with
Total organic Carbon removal is represented)
Above result shows, influence of the dosage to coagulation effect greatly, TOC clearances with processing basicity and
The change of PZC dosages and change.When basicity is 1.0 and 1.5, under the dosage in addition to 20mg/L, TOC clearances are equal
It is high during than B=0.Maximum TOC removal efficiency is obtained when basicity and PZC dosages are respectively 1.5 and 15mg/L, is
48.8%.In optimal conditions, remaining TOC concentration is reduced to 4.44mg/L from 8.68mg/L, is respectively equivalent to 34.72 Hes
17.76mg COD/L (are worth to) according to TOC in municipal wastewater and COD empirical relation, illustrate do not adjusting the feelings of pH value
PZC coagulations can significantly improve effluent quality under condition.
Application example 3
N2 (B=0.5) polymerization zirconium chloride inorganic polymer coagulants prepared by above example 1 are used for humic garden sorrel
Intend the processing of waste water, study the coagulation effect for polymerizeing zirconium chloride under condition of different pH, dosage is 10mg/L.Coagulation effect
Represented with total organic Carbon removal, result is listed in such as table 4 below.
It polymerize treatment effect of the zirconium chloride inorganic polymer coagulant to humic acid simulated wastewater under the condition of different pH of table 4
(being represented with total organic Carbon removal)
When dosage is 10mg/L, HA clearances highest when pH scopes are 7-9, is 96%.These results indicate that zirconium is mixed
Solidifying agent has specific requirement to obtain preferable coagulation effect under given dosage to pH.
Although the present invention is described with reference to above example, the present invention is not limited to above-described embodiment,
And be only defined by the appended claims, those of ordinary skill in the art easily can modify and change to it, but simultaneously
Without departing from the essential idea and scope of the present invention.
Claims (10)
1. a kind of preparation method for polymerizeing zirconium chloride inorganic polymer coagulant, it is as follows that methods described includes step：
(1) 10%-20% (w/v) ZrCl is configured with deionized water4Solution；
(2) at 0-4 DEG C, by ZrCl4Solution is under conditions of stir speed (S.S.) is 300-800rpm stirring, by concentration in 80-
200g/L concentrated alkali solution is added slowly to ZrCl4In solution so that basicity is in the range of more than 0 to 2.5, wherein basicity
=[OH-]/[Zr4+]；
(3) above-mentioned steps (2) concentrated alkali solution adding procedure is according to the difference of basicity, and addition time control is within 3h, then
Continue to stir 3-5h, obtain transparent clarification and in the absence of the solution of visible precipitate thing, that is, the polymerization tetrachloro of different basicities is made
Change zirconium inorganic polymer coagulant solution.
2. the preparation method of polymerization zirconium chloride inorganic polymer coagulant according to claim 1, wherein, in step
(1) in, use quality concentration is 98%-100% ZrCl4It is configured to described ZrCl4Solution.
3. the preparation method of polymerization zirconium chloride inorganic polymer coagulant according to claim 1, wherein, step (2)
Described in predetermined basicity be 0.2-2.5.
4. the preparation method of polymerization zirconium chloride inorganic polymer coagulant according to claim 1, wherein the concentrated base
Solution is selected from sodium hydroxide solution and potassium hydroxide solution.
5. the preparation method of polymerization zirconium chloride inorganic polymer coagulant according to claim 1, wherein, in step
(2) in, concentrated alkali solution is added in the way of being added dropwise to the ZrCl prepared by step (1)4In solution.
6. the zirconium chloride inorganic macromolecule compound that a kind of method according to any one of claim 1-5 is obtained.
7. the polymerization zirconium chloride inorganic polymer coagulant that the method according to any one of claim 1-5 is obtained is in water
The purposes of water treatment agent is used as in processing.
8. purposes according to claim 7, the purposes includes preparing the method any one of claim 1-6
The polymerization zirconium chloride inorganic polymer coagulant of acquisition is directly appended to need in water to be processed or sewage.
9. purposes according to claim 7, wherein, the dosage of the polymerization zirconium chloride inorganic polymer coagulant is
10-40mg/ rises water or sewage, and the pH scopes of the water or waste water are 4-10.
10. purposes according to claim 8, it is described need to water or sewage to be processed include feedwater, drinking water or from making
Waste water in paper, mining, textile printing and dyeing and filed of daily-use chemical industry.
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| CN108083399A (en) * | 2017-12-21 | 2018-05-29 | 北京工业大学 | A kind of method for being classified enhanced coagulation |
| CN108128864A (en) * | 2017-12-21 | 2018-06-08 | 北京工业大学 | A kind of preparation method of polyaluminium zirconium aluminium inorganic high efficient flocculant |
| CN108128863A (en) * | 2017-12-21 | 2018-06-08 | 北京工业大学 | A kind of preparation method of polymeric silicicacid polyaluminium zirconium inorganic polymer flocculant |
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| CN102976462A (en) * | 2012-12-20 | 2013-03-20 | 山东大学 | Polymerized titanium tetrachloride inorganic polymeric flocculant and preparation method of inorganic polymeric flocculant |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108083399A (en) * | 2017-12-21 | 2018-05-29 | 北京工业大学 | A kind of method for being classified enhanced coagulation |
| CN108128864A (en) * | 2017-12-21 | 2018-06-08 | 北京工业大学 | A kind of preparation method of polyaluminium zirconium aluminium inorganic high efficient flocculant |
| CN108128863A (en) * | 2017-12-21 | 2018-06-08 | 北京工业大学 | A kind of preparation method of polymeric silicicacid polyaluminium zirconium inorganic polymer flocculant |
| WO2019119477A1 (en) * | 2017-12-21 | 2019-06-27 | 北京工业大学 | Preparation method for polymeric zirconium aluminum chloride inorganic high-efficiency flocculant |
| CN108128863B (en) * | 2017-12-21 | 2019-08-09 | 北京工业大学 | A kind of preparation method of polymeric silicicacid polyaluminium zirconium inorganic polymer flocculant |
| US20210032114A1 (en) * | 2017-12-21 | 2021-02-04 | Beijing University Of Technology | A Method of Preparing Inorganic Macromolecular Flocculant by Polymerizing Silicate and Zirconium Chloride |
| US11492263B2 (en) * | 2017-12-21 | 2022-11-08 | Beijing University Of Technology | Method of preparing inorganic macromolecular flocculant by polymerizing silicate and zirconium chloride |
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