CN102040293B - Method and device for purifying high-fluorine underground water - Google Patents
Method and device for purifying high-fluorine underground water Download PDFInfo
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- CN102040293B CN102040293B CN 200910235468 CN200910235468A CN102040293B CN 102040293 B CN102040293 B CN 102040293B CN 200910235468 CN200910235468 CN 200910235468 CN 200910235468 A CN200910235468 A CN 200910235468A CN 102040293 B CN102040293 B CN 102040293B
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Abstract
The invention relates to a method for purifying high-fluorine underground water, which comprises the following steps of: removing fluorine ions from the high-fluorine underground water by an adsorption method, and performing ion exchange. The device mainly comprises a fluorine removing unit and a security ion exchange unit, wherein the fluorine removing unit is provided with at least one fluorine removing absorption tank in which a filler is arranged; the filler is an adsorbent and adsorbs the fluorine ions in raw water; the security ion exchange unit is provided with an ion exchange tank and is connected in series with the fluorine removing unit; and a filler is arranged in the ion exchange unit, is resin and removes metal cations from the raw water. The fluorine removing unit removes the fluorine ions from the high-fluorine underground water through adsorption, and the security ion exchange unit removes other metal cations which exceed the standard from the high-fluorine underground water. The water quality of effluent after the high-fluorine underground water is treated by the method can reach the standard.
Description
Technical field
The invention belongs to application field of water treatment, specifically, relate to a kind of high fluorine groundwater purifying method.
The invention still further relates to a kind of device for realizing aforesaid method.
Background technology
Fluorine is one of trace element of needed by human, then causes poisoning but intake is too high.Country has formulated strict standard (1mg/L) (GB5749-2006) to fluorine content in the tap water.The approach that human body is taken in fluorine mainly contains tap water, food, air, and wherein tap water is main path.Drinking the fluorine disease that water of high fluorine content causes is the most widely one of the endemy that distributes in the world, and the countries such as Argentina, the U.S., Morocco, India, China are all relevant for the report of endemic fluorine poisoning in the world, and are wherein serious with India and the China in Asia.China is except upper overseas, and all the other each province, autonomous region and municipality directly under the Central Government find that all the drinking water type fluorine is sick, and be comparatively serious with northeast, North China, northwest, Beijing, Tianjin.According to Department of Disease Control of Ministry of Health statistics in 2004, totally 1117 in the county that national drinking water type fluorosis occurs, high fluorine exposure (>1.0mg/L) population reaches 8,141 ten thousand.China is carrying out many work aspect solution high fluorice region, the rural area drinking water safety guarantee.The Eleventh Five-Year Plan period Ministry of Water Resources has started " construction of rural potable water safety control demonstration county " work, but still to beat deep-well, to look for the schemes such as new water source or remote water transfer as main, these methods are subject to respectively many condition restriction such as source quality condition, local ground watering margin, shut-in well technology, the sparsely populated degree in village, operational management at present.Especially for outlying Rural areas, in the urgent need to safe, the effective technology of Fluoride Removal for existing water source.
The method of drinking water defluorination has coagulant sedimentation, absorption method, ion exchange method, membrane separation process, electroosmose process, electrocoagulation etc., and wherein absorption method is comparatively economical and practical.The sorbent material that various countries generally adopt has activated alumina, bone black etc., but loading capacity is all lower, and there is applicable pH slant acidity (4.5-5.5) in activated alumina, and aluminum ion is easy to stripping, the low easily shortcoming such as broken of granule strength.
Some results of study in recent years show, polyvalent metal (hydration) oxide compounds such as aluminium, magnesium, iron, zirconium and rare earth have preferably Adsorption of fluoride performance.It has structural porosity, iso-electric point advantages of higher, can when suitable pH the mineral surface hydroxylation occur form a series of metal hydroxidess and poly-hydroxy hydrous metal oxides, the existence of surface hydroxyl function base makes it to have powerful avidity, changes absorption by covalent linkage chemisorption electrostatic adhesion and ion and waits that effect is adsorbed, fixing fluorochemical.
Jiao Zhongzhi, Zhang Yu, Yang Min etc. are in " the inorganic synthetic materials of cerium base is to the Study on adsorption properties of fluorine " (environmental chemistry, Vol21, No.4,2002) reported in the Chinese that utilization iron-based rare-earth matrix material is used for defluorination, adsorptive capacity to fluorine in the scope of pH 3-5 is higher, and is lower in normal tap water pH6.5-8.5 scope internal adsorption performance.
Yang Min, Wu Xiaomei, Zhang Yu in Chinese patent " a kind of composite oxides de-fluoridation adsorbent " (patent No. ZL200510116751.0), reported a kind of under neutrallty condition to the saturated extent of adsorption of the fluorine sorbing material up to 179mg/g.
But, directly use powder sorbent not have practicality, because directly being added to the water, powder can cause a large amount of losses, cause hydro-colloid or turbidity to exceed standard, droop loss is large, obstruction, can not ensure continuous effluent, should make it become particle by powder technology, fill in the absorbing unit, be conducive to adsorb saturated rear regeneration and reuse the reduction cost.In addition, because may also existing other concentration of metal ions outside defluorination, the arsenic to exceed standard in the underground water, as: Fe, Mn, Cu, Cr, Cd, Pb etc., the sorbent material life-time service also may have the micro-metals stripping, need to remove by resin absorption in security personnel's ion-exchange unit, guarantee permeate safety.In addition, on the basis of adsorption-defluorination unit and security personnel's ion-exchange unit combination, also need cooperate disinfecting of preoxidation to water inlet/sterilization and water outlet, and the optimization operating parameter, the strong Removal of Fluorine From Underground Water safety water supply equipment of suitability could be formed.In addition, this technique also can solve this accidental when envrionment conditions great change sorbent material trace metal stripping problem
Therefore, the key that promotes this sorbent material application is defluorination method and the device that exploitation is applicable to this absorption, carries out high fluorine groundwater and processes, and guarantee permeate safety.
Summary of the invention
The purpose of this invention is to provide a kind of high fluorine groundwater purifying method.
Another purpose of the present invention provides a kind of device for realizing aforesaid method.
For achieving the above object, high fluorine groundwater purifying method provided by the invention, first with high fluorine groundwater by being filled with the defluorination unit of composite oxides de-fluoridation adsorbent particle, in the Adsorption water behind the fluorion, through being filled with security personnel's ion-exchange unit of ion exchange resin, carry out ion-exchange again.
The composite oxides de-fluoridation adsorbent particle that the present invention adopts, it is the composite metal oxide adsorbent powder that provides according to Chinese patent ZL200510116751.0, adding the particle that the high polymer binder extrinsion pressing makes (is a known technology with the powder granulation again, and not the emphasis that the present invention discusses, therefore be not described in detail).
The composite oxides de-fluoridation adsorbent that Chinese patent ZL200510116751.0 provides is comprised of transition metal, Al and rare earth metal, and wherein: the mol ratio of transition metal, Al and rare earth metal is 0.5-1.5: 2-6: 0.5-1.5; Transition metal is Ti, V, Cr, Mn, Fe, Co, Ni, Cu or Zn;
The ion exchange resin that the present invention adopts is macroporous chelate resin or storng-acid cation exchange resin.
In the method for the present invention, can also in absorption method removal water before the fluorion, carry out oxidation to high fluorine groundwater, to suppress microbial growth in the water, oxidation is as oxygenant with dioxide peroxide, clorox or ozone.
In the method for the present invention, can also comprise the water outlet after filtering is carried out disinfection, sterilization is or/and uviolizing with clorox, ozone.
Device for realizing aforesaid method provided by the invention mainly comprises:
The defluorination unit has at least one defluorination adsorption tanks, in filler is housed, this filler is composite oxides de-fluoridation adsorbent particle, adsorbs the fluorion in the former water;
Security personnel's ion-exchange unit has an ion exchange pot, is connected with defluorination cell string mode, and filler is housed in the ion-exchange unit, and this filler is resin, removes the metallic cation in the former water.
In the device of the present invention, the defluorination unit comprises:
The preoxidation device of microbial growth in the preposition inhibition water is equipped with dioxide peroxide, clorox or ozone oxidation agent in this preoxidation device;
Preposition former water reserve tank and reducing valve;
In the device of the present invention, security personnel's ion-exchange unit comprises:
Rearmounted one processes the water reserve tank, is used for defluorination unit and security personnel's ion-exchange unit are carried out back flushing.
In the device of the present invention, the defluorination unit can adopt fixed bed, and sorbent material is composite oxides de-fluoridation adsorbent particle.
In the device of the present invention, security personnel's ion-exchange unit can adopt fixed bed, and the resin that is equipped with in this security personnel's ion-exchange unit is polystyrene resin D401Styrene-DVB and D418Styrene-DVB, polystyrene thiol resin D402Styrene-DVB, storng-acid cation exchange resin 001 * 7Styrene-DVB, 002 * 7Styrene-DVB, 001 * 8Styrene-DVB, 001 * 7 * 7Styrene-DVB or weakly acidic cation-exchange resin 110Acreylic-DVB, D113Acreylic, DLT-1Sryrene-DVB.
In the device of the present invention, the defluorination unit is 3 with the filler Intake Quantity volume ratio of security personnel's ion-exchange unit: 1-10: 1.
In the device of the present invention, also comprise a regeneration unit, the sorbent material after the defluorination unit passes is regenerated.
The present invention is by the process combination of adsorption-defluorination unit with security personnel's ion-exchange unit, fluorion in the high fluorine groundwater is removed in design, remove simultaneously the device that contains other metal ion that exceeds standard in the water, make water quality reach " drinking water sanitary standard " requirement (GB5749-2006).
Description of drawings
Fig. 1 is that the present invention is for the treatment of the schema of high fluorine groundwater method.
Fig. 2 is that the present invention is for the treatment of the device schematic diagram of high fluorine groundwater.
Fig. 3 is embodiment 1-5 concentration schematic diagram of fluorine in the water outlet under different water flowing multiplying powers.
Embodiment
In conjunction with Fig. 1 and Fig. 2, be that the process flow diagram of defluorination of the present invention and the present invention are for the treatment of the device schematic diagram of high fluorine groundwater.
The present invention includes following processing unit:
The former water of high fluorine groundwater is fluorion in defluorination unit Adsorption water, can remove the arsenic acid negatively charged ion simultaneously.The defluorination unit adopts fixed bed, filler is composite oxides de-fluoridation adsorbent particle, it is a kind of composite metal oxide adsorbent powder that provides according to Chinese patent ZL200510116751.0, make the particle that particle diameter is 0.5-1.7mm, preferable particle size 0.7-1.3mm by adding the high polymer binder extrinsion pressing.SV is 3-30h when processing high fluorine groundwater
-1
The defluorination unit can arrange 1-4 adsorption tanks, regularly or the level pressure recoil, regenerates after penetrating or changes filler.If the defluorination unit arranges 1 adsorption tanks, can adopt intermittent operation.If described defluorination unit is comprised of 2-4 adsorption tanks, can adopt alternate run, simultaneously the operation adsorption tanks can adopt the series winding or and the mode that connects connect.The defluorination unit can also connect regeneration unit, and the adsorption tanks after the defluorination unit passes are regenerated.
The water outlet of defluorination unit enters security personnel's ion-exchange unit, mainly removes to contain other metallic cation that exceeds standard in the water.
The defluorination unit is connected with serial arrangement with security personnel's ion-exchange unit.Security personnel's ion-exchange unit adopts fixed bed, and to stream, filler is that resin is macroporous chelate resin or storng-acid cation exchange resin under selecting.Macroporous chelate resin is macropore polystyrene resin D401Styrene-DVB and D418Styrene-DVB or macropore polystyrene thiol resin D402Styrene-DVB.Storng-acid cation exchange resin is such as being: 001 * 7Styrene, 002 * 7Styrene, 001 * 8Styrene, 001 * 7 * 7Styrene; Weakly acidic cation-exchange resin is such as being: 110Acreylic-DVB, D113Acreylic, DLT-1Sryrene-DVB.
The defluorination unit is 3 with the amount of filler volume ratio of security personnel's ion-exchange unit: 1-10: 1.
Can set up former water reserve tank and reducing valve before the defluorination unit, but set handling water reserve tank behind security personnel's ion-exchange unit uses the water of processing in the water water tank that defluorination unit and security personnel's ion-exchange unit are carried out back flushing.
Different according to raw water quality, can before entering treatment system, set up Yuan Shui the preoxidation device, be used for suppressing the water microbial growth, prevent system jams.Oxygenant is dioxide peroxide or clorox or ozone.
Security personnel's ion-exchange unit water outlet can carry out disinfection as required, and sterilizing agent is that clorox or ozone are or/and ultraviolet.
The below is described in detail the present invention, and in detailed description, its implication of the shortenings of employing is:
The empty bed of SV-speed refers to that the flow by adsorption bed is what times of adsorption bed volume in the unit time, and unit is h
-1
BV-water flowing multiplying power refers to that the water yield (by volume) of processing is what times of adsorption bed volume, dimentionless quantity.
Embodiment 1
Filler in the defluorination unit adsorption tanks is the complex metal oxides particle, and 3 filler is the D418 resin in security personnel's ion-exchange unit.Former water be adopt tap water to add Sodium Fluoride (NaF) to be mixed with fluorine concentration be 5.5mg/L, initial pH=7.7.
Former water is with SV=3h
-1Process through defluorination unit and security personnel's ion-exchange unit successively, former water and each unit effluent quality are seen Fig. 3 and table 1 (fluorinion concentration measuring method: ion selective electrode method, other concentration of metal ions measuring method can adopt ICP-OES or ICP-MS):
Table 1 (unit: mg/L)
Former water | The defluorination unit | Rearmounted filtering unit | |
Fe | N.D. | N.D. | N.D. |
Mn | N.D. | N.D. | N.D. |
Cu | 0.001 | 0.001 | N.D. |
Cr | N.D. | N.D. | N.D. |
Cd | N.D. | N.D. | N.D. |
Pb | N.D. | N.D. | N.D. |
Ca | 61.62 | 62.02 | 59.66 |
Al | 0.035 | 0.056 | 0.044 |
La | N.D. | N.D. | N.D. |
Ce | N.D. | N.D. | N.D. |
As shown in Figure 3, the following water outlet fluorine of 2100BV volume concentration<1mg/L reaches " drinking water sanitary standard " (GB5749-2006).
By as seen from Table 1, each concentration of metal ions of water outlet of processing through the present invention all reaches " drinking water sanitary standard " (GB5749-2006).
Embodiment 2
Filler in the defluorination unit adsorption tanks is the complex metal oxides particle, and the filler in security personnel's ion-exchange unit is the D401 resin.Former water be adopt tap water to add Sodium Fluoride (NaF) to be mixed with fluorine concentration be 5.5mg/L, initial pH=7.7 transfers to pH=7.0 with hydrochloric acid.
Former water is with SV=30h
-1Process through defluorination unit and security personnel's ion-exchange unit successively, former water and each unit effluent quality are seen Fig. 3 and table 2 (fluorinion concentration measuring method: ion selective electrode method, other concentration of metal ions measuring method can adopt ICP-OES or ICP-MS):
Table 2 (unit: mg/L)
Former water | The defluorination unit | Rearmounted filtering unit | |
Fe | N.D. | N.D. | N.D. |
Mn | N.D. | N.D. | N.D. |
Cu | N.D. | N.D. | N.D. |
[0059]
Cr | N.D. | N.D. | N.D. |
Cd | N.D. | N.D. | N.D. |
Pb | N.D. | N.D. | N.D. |
Ca | 60.05 | 59.54 | 59.46 |
Al | 0.033 | 0.087 | 0.032 |
La | N.D. | N.D. | N.D. |
Ce | N.D. | 0.120 | N.D. |
As shown in Figure 3, the following water outlet fluorine of 900BV volume concentration<1mg/L reaches " drinking water sanitary standard " (GB5749-2006).
By as seen from Table 2, each concentration of metal ions of water outlet of processing through the present invention all reaches " drinking water sanitary standard " (GB5749-2006).
Embodiment 3
Filler in the defluorination unit adsorption tanks is the complex metal oxides particle, and the filler in security personnel's ion-exchange unit is the D418 resin.Former water be adopt tap water to add Sodium Fluoride (NaF) to be mixed with fluorine concentration be 5.5mg/L, initial pH=7.7 transfers to pH=5.0 with hydrochloric acid.
Former water is with SV=5h
-1Process through defluorination unit and security personnel's ion-exchange unit successively, former water and each unit effluent quality are seen Fig. 3 and table 3 (fluorinion concentration measuring method: ion selective electrode method, other concentration of metal ions measuring method can adopt ICP-OES or ICP-MS):
Table 3 (unit: mg/L)
Former water | The defluorination unit | Rearmounted filtering unit | |
Fe | N.D. | N.D. | N.D. |
Mn | N.D. | N.D. | N.D. |
Cu | 0.002 | 0.002 | N.D. |
Cr | N.D. | N.D. | N.D. |
Cd | N.D. | N.D. | N.D. |
Pb | N.D. | N.D. | N.D. |
Ca | 60.67 | 60.58 | 60.43 |
Al | 0.041 | 0.058 | 0.033 |
[0067]
La | N.D. | N.D. | N.D. |
Ce | N.D. | 0.323 | N.D. |
As shown in Figure 3, the following water outlet fluorine of 830BV volume concentration<1mg/L reaches " drinking water sanitary standard " (GB5749-2006).
By as seen from Table 3, each concentration of metal ions of water outlet of processing through the present invention all reaches " drinking water sanitary standard " (GB5749-2006).
Embodiment 4
Filler in the defluorination unit adsorption tanks is the complex metal oxides particle, and the filler in security personnel's ion-exchange unit is resin 002 * 7 Styrene-DVB.Former water is to adopt certain village's high fluorine groundwater, and fluorine concentration is 2.07mg/L, pH=7.8.
Use first 10BV and SV=10h
-1Tap water clean the defluorination unit, then former water is with SV=20h
-1Process through defluorination unit and security personnel's ion-exchange unit successively, former water and each unit effluent quality are seen Fig. 3 and table 4 (fluorinion concentration measuring method: ion selective electrode method, other concentration of metal ions measuring method: ICP-OES, ICP-MS):
Table 4 (unit: mg/L)
Former water | The defluorination unit | Rearmounted filtering unit | |
Fe | 1.56 | 1.49 | 0.095 |
Mn | 0.046 | 0.044 | 0.001 |
Cu | 0.001 | 0.001 | N.D. |
Cr | N.D. | N.D. | N.D. |
Cd | 0.00098 | 0.00097 | N.D. |
Pb | N.D. | N.D. | N.D. |
Ca | 49.55 | 49.34 | 48.99 |
Al | 0.035 | 0.056 | 0.027 |
La | N.D. | N.D. | N.D. |
Ce | N.D. | N.D. | N.D. |
As shown in Figure 3, the following water outlet fluorine of 1760BV volume concentration<1mg/L reaches " drinking water sanitary standard " (GB5749-2006).
By as seen from Table 4, each concentration of metal ions of water outlet of processing through the present invention all reaches " drinking water sanitary standard " (GB5749-2006).
Embodiment 5
Filler in the defluorination unit adsorption tanks is the complex metal oxides particle, and the filler in security personnel's ion-exchange unit is DLT-1 Sryrene-DVB resin.Former water is to adopt certain village's high-arsenic underground water, and arsenic concentration is 0.065mg/L, pH=7.4.
Use first 10BV and SV=10h
-1Tap water clean the defluorination unit, then former water is with SV=5h
-1Process through defluorination unit and security personnel's ion-exchange unit successively, former water and each unit effluent quality are seen Fig. 4 and table 5 (fluorinion concentration measuring method: ion selective electrode method, other concentration of metal ions measuring method: ICP-OES, ICP-MS):
Table 5 (unit: mg/L)
Former water | The defluorination unit | Rearmounted filtering unit | |
Fe | 1.07 | 1.49 | 0.095 |
Mn | 2.05 | 0.044 | 0.001 |
Cu | 0.015 | 0.013 | N.D. |
Cr | N.D. | N.D. | N.D. |
Cd | N.D. | N.D. | N.D. |
Pb | N.D. | N.D. | N.D. |
Ca | 63.10 | 62.89 | 61.9 |
Al | 0.046 | 0.055 | 0.030 |
La | N.D. | N.D. | N.D. |
Ce | N.D. | N.D. | N.D. |
As shown in Figure 4, the following water outlet arsenic concentration<0.010mg/L of 10300BV volume reaches " drinking water sanitary standard " (GB5749-2006).
By as seen from Table 5, each concentration of metal ions of water outlet of processing through the present invention all reaches " drinking water sanitary standard " (GB5749-2006).
Claims (8)
1. high fluorine groundwater purifying method, first high fluorine groundwater is carried out pre-oxidation treatment, to suppress microbial growth in the water, then with high fluorine groundwater by being filled with the defluorination unit of composite oxides de-fluoridation adsorbent particle, in the Adsorption water behind the fluorion, through being filled with security personnel's ion-exchange unit of ion exchange resin, carry out ion-exchange again;
Described composite oxides de-fluoridation adsorbent is comprised of transition metal, Al and rare earth metal, wherein:
The mol ratio of transition metal, Al and rare earth metal is 0.5-1.5: 2-6: 0.5-1.5;
Transition metal is Ti, V, Cr, Mn, Fe, Co, Ni, Cu or Zn;
Ion exchange resin is macroporous chelate resin or storng-acid cation exchange resin;
The defluorination unit is 3 with the amount of filler volume ratio of security personnel's ion-exchange unit: 1-10: 1.
2. high fluorine groundwater purifying method as claimed in claim 1 wherein, is series connection between defluorination unit and the ion-exchange unit.
3. high fluorine groundwater purifying method as claimed in claim 1 or 2, wherein, the defluorination unit is single or multiple fixed bed serial or parallel connections.
4. high fluorine groundwater purifying method as claimed in claim 1 or 2, wherein, security personnel's ion-exchange unit is fixed bed.
5. high fluorine groundwater purifying method as claimed in claim 1, wherein, ion exchange resin is polystyrene resin, polystyrene thiol resin, storng-acid cation exchange resin or weakly acidic cation-exchange resin.
6. high fluorine groundwater purifying method as claimed in claim 1, wherein, the oxygenant that pre-oxidation treatment adopts is dioxide peroxide, clorox or ozone.
7. high fluorine groundwater purifying method as claimed in claim 1 wherein, is passed through the again disinfection of water outlet that security personnel's ion-exchange unit is processed.
8. high fluorine groundwater purifying method as claimed in claim 7, wherein, the sterilizing agent of disinfecting employing is clorox or ozone.
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CN104843818B (en) * | 2015-05-21 | 2017-11-10 | 台湾化学纤维股份有限公司 | The defluorination method and its fluorine removal device of fluoride waste |
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CN1954906A (en) * | 2005-10-28 | 2007-05-02 | 中国科学院生态环境研究中心 | Compound metal oxide de-fluorine sorbent |
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