CN103241858A - Reaction tank, processing device and processing method thereof - Google Patents
Reaction tank, processing device and processing method thereof Download PDFInfo
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- CN103241858A CN103241858A CN2013100511623A CN201310051162A CN103241858A CN 103241858 A CN103241858 A CN 103241858A CN 2013100511623 A CN2013100511623 A CN 2013100511623A CN 201310051162 A CN201310051162 A CN 201310051162A CN 103241858 A CN103241858 A CN 103241858A
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Abstract
The invention relates to a reaction tank, a processing device and a processing method thereof, wherein by means of the reaction tank, fluorine in the water can be simply and efficiently removed to ensure the water permeability for a long time, while used reagents can be recovered simply and efficiently. The reaction tank can be used for removing fluorine in a fluorine-containing object. The reaction tank is characterized by containing sands and reactants, wherein a first layer of sands, a reactant layer and a second layer of sands are sequentially formed at the upper part of the reaction tank by the sands and the reactants. The reactants contain calcium hydrogen phosphate dehydrate (a) and particles (b), wherein the calcium hydrogen phosphate dehydrate (a) is loaded on the particles (b).
Description
[technical field]
The present invention relates to for the reactive tank of removing fluorine from the processing object water that contains fluorine, possess the treatment facility of this reactive tank and use this reactive tank to remove the method for fluorine.
[background technology]
The draining of discharging in the matting by electric components such as the pickling process of the manufacturing process of the electrorefining operation of aluminium, phosphatic manure, stainless steel etc., silicon or waste incineration field are washed and are contained fluorine in cigarette draining, the coal firepower stack desulfurization draining etc., in order to suppress these fluorine to the influence of environment, need remove it.
In patent documentation 1, proposed following apparatus, in this device, contacted with the crystal seed that is constituted by fluorine and calcium by making fluorine-containing draining, the fluorine generation crystallization in the draining is removed.Specifically, wherein put down in writing a kind for the treatment of unit of fluorine-containing draining, its for have from coexistence calcium simultaneously fluorine concentration be the fluorine-containing drain treatment apparatus that the draining of lower concentration of 10mg/L～15mg/L fluorine generation crystallization is removed, it is characterized in that above-mentioned treatment unit possesses: the crystallization reactive tank that is filled with a large amount of crystal seeds; Flow unit (means) makes above-mentioned draining flow into, make simultaneously a part of handling water to circulate from the below of above-mentioned crystallization reactive tank, thereby forms the fluidized-bed of crystal seed in above-mentioned crystallization reactive tank; Medicament injects the unit, injects the crystallization with medicament that contains phosphoric acid in above-mentioned crystallization reactive tank; Fluorine concentration determination unit, the fluorine concentration of the processing water of handling to above-mentioned draining or through above-mentioned crystallization reactive tank is measured; The injection rate control unit, by the measurement result of above-mentioned fluorine concentration determination unit, the difference of the fluorine concentration of the processing water after handling through above-mentioned crystallization reactive tank and the fluorine concentration of above-mentioned draining is in the injection rate that can not surpass the above-mentioned crystallization with medicament of scope inner control of prescribed value; The pH determination unit is measured the pH in the above-mentioned crystallization reactive tank; The pH adjustment unit is adjusted to specialized range based on the measured value of above-mentioned pH determination unit with the pH in the above-mentioned crystallization reactive tank.As above-mentioned crystal seed, use the crystal seed that is constituted by hydroxyapatite and calcium phosphate.
As the reagent that is used for removing fluorine, in patent documentation 2, put down in writing following reagent, this reagent is characterised in that it contains dicalcium phosphate dihydrate (A) and particle (B), dicalcium phosphate dihydrate (A) is carried on particle (B).
[prior art document]
[patent documentation]
Patent documentation 1: TOHKEMY 2005-246318 communique
Patent documentation 2: the international brochure that discloses No. 2010/134573
[summary of the invention]
[inventing problem to be solved]
In the treatment unit that patent documentation 1 is put down in writing, by fluorine-containing draining is contacted with the crystal seed that is made of hydroxyapatite and calcium phosphate, make the fluorine in the draining produce crystallization at crystal seed, but have the carrying out along with crystallization, the problem that crystal seed solidifies, the water-permeable reduction is such occurs.In addition, solidify because crystal seed produces, thereby have the problem that when it is exchanged, is difficult to from reactive tank, extract out.
In patent documentation 2, put down in writing and contained dicalcium phosphate dihydrate (A) and particle (B), dicalcium phosphate dihydrate (A) by the reagent of particle (B) load, but itself and unexposed concrete form used when being applied to actual treatment equipment.
The object of the present invention is to provide a kind of reactive tank, its can solve above-mentioned existing problem, can be easy and efficient remove fluorine in the draining well, can guarantee water-permeable for a long time simultaneously, further can be easy and the reagent of high-recovery ground after to use reclaim.
[solving the means of problem]
The inventor is conceived to the formation of removing the reactive tank of fluorine for from processing object water for having carried out various researchs for the method for removing fluorine from the processing object water that contains fluorine.And find, by adopting the reactive tank of following formation, can be easy and efficient from the processing object water that contains fluorine, remove fluorine well, can guarantee water-permeable for a long time simultaneously, further can be easy and the reagent of high-recovery ground after to use reclaim; In this reactive tank, make reactive tank have first layer of sand, reagent layer and second layer of sand successively from top; The reagent that the reagent layer contains contains dicalcium phosphate dihydrate (A) and particle (B), and dicalcium phosphate dihydrate (A) is by particle (B) load; First layer of sand is formed by first sand of effective diameter less than particle (B); Second layer of sand is formed by second sand of effective diameter less than particle (B).So expect, can thoroughly solve above-mentioned problem as reactive tank by the device that use has a specific formation, thereby finish the present invention.
Namely, the present invention relates to a kind of reactive tank, it is for being used for removing from the processing object water that contains fluorine the reactive tank of fluorine, wherein, accommodate sand and reagent in above-mentioned reactive tank, above-mentioned sand and above-mentioned reagent constitute first layer of sand, reagent layer and second layer of sand successively from the top of above-mentioned reactive tank; Above-mentioned reagent contains dicalcium phosphate dihydrate (A) and particle (B), and dicalcium phosphate dihydrate (A) is by particle (B) load; Above-mentioned first layer of sand is made up of less than first sand of above-mentioned particle (B) effective diameter; Above-mentioned second layer of sand is made up of less than second sand of above-mentioned particle (B) effective diameter.
[effect of invention]
Reactive tank of the present invention is owing to be made of to form above-mentioned, thus can be easy and efficient remove fluorine in the draining well, can guarantee water-permeable for a long time simultaneously, further can be easy and the reagent of high-recovery ground after to use reclaim.
[description of drawings]
Fig. 1 is the synoptic diagram that briefly shows an example of the treatment facility that possesses reactive tank of the present invention.
Fig. 2 is the schematic cross-section of the reactive tank of making example 1 record.
Fig. 3 is the synoptic diagram that briefly shows the treatment facility of making example 1 record.
[embodiment]
The present invention is described in detail in detail below.
Reactive tank of the present invention is for being used for removing from the processing object water that contains fluorine the reactive tank of fluorine.Accommodate sand and reagent in the reactive tank of the present invention, contact with reagent in the process to the bottom circulation by making the processing object water that injects from the top of reactive tank, fluorine is fixed in the reagent and removes fluorine from processing object water.(hereinafter also simply be called " processing water " by from handle object water, removing the processing water that fluorine obtains with contacting of reagent.) from water port, discharge.
The shape of above-mentioned reactive tank, size, material etc. are not particularly limited, and can (hereinafter also simply be called " fluorine concentration " according to the fluorinion concentration of the treatment capacity of handling object water, processing object water.) wait suitably and determine.As the shape of groove, can enumerate for example cylindric, case shape etc.As the material of groove, can enumerate for example plastics, vinylchlorid, acrylic, resin, metal etc.
Reactive tank of the present invention is owing to have above-mentioned formation, thereby reagent does not solidify, the water-permeable excellence.
In the reactive tank of the present invention, hold sand and reagent by the mode that constitutes at least 3 layers, from the top of groove, be provided with first layer of sand, reagent layer and second layer of sand successively.Handling object water handles by first layer of sand, reagent layer, second layer of sand successively.Thereby, reactive tank of the present invention can be easy and efficient remove fluorine in the draining well, can guarantee water-permeable for a long time simultaneously, further can prevent the outflow of reagent, thus can be easy and the reagent of high-recovery ground after to use reclaim.
For example, people also consider to use net to wait to prevent the loss of reagent, but net can be gradually deterioration, and the operability under introducing (Guide goes into) situation in the practicality equipment is poor, is difficult to change operation.
For each layer, adjacent 2 layers boundary can be indeterminate, can have to constitute the zone that this composition of 2 layers mixes between adjacent 2 layers.For example, between first layer of sand and reagent layer, can have the zone that first sand and reagent mix.
The thickness of reagent layer is not particularly limited, and can suitably set according to the treatment capacity of processing object water, the fluorine concentration of processing object water etc., to realize the fluorine amount of removing of the phase of being hoped.For example be preferably more than the 30cm.
Above-mentioned reagent contains dicalcium phosphate dihydrate (A) and particle (B) (particle that does not wherein comprise dicalcium phosphate dihydrate (A)), and dicalcium phosphate dihydrate (A) is by particle (B) load.The particle diameter of preferred particulates (B) is greater than dicalcium phosphate dihydrate (A) powder.
Dicalcium phosphate dihydrate (A) reacts with the fluorine that processing object water contains, and generates Ca
10(PO
4)
6F
2Represented fluorapatite.Thus, the fluorine of removing is immobilized with the form of fluorapatite and is insoluble, thus not stripping again.
In the fluorapatite, natural Rock Phosphate (72Min BPL) etc. are principal constituent, in reactive tank of the present invention, needn't use other organic substance or heavy metal class etc.Thereby, by using above-mentioned reagent, can not cause secondary environmental pollution, can be by simple operation economy and reduce to handle the fluorine concentration of object water reliably.
About above-mentioned reagent, in order to improve the efficient of removing of fluorine, even under the situation of the micropowder of selecting dicalcium phosphate dihydrate (A), also can be by selecting the bigger particle (B) of particle diameter ratio, making dicalcium phosphate dihydrate (A) be carried on the particle diameter of its augmenting response agent that comes up, thereby reagent is difficult for glomeration (ダ マ, agglutinator), can form the reagent layer of water-permeable excellence.And under the situation of the powder that uses separately dicalcium phosphate dihydrate, no matter its particle diameter how, the powder of dicalcium phosphate dihydrate all can solidify, water-permeable reduces, and this tendency is that particle diameter is more little more remarkable.
In addition, owing to above-mentioned reagent is made of dicalcium phosphate dihydrate (A) and particle (B), thereby compare with the situation of independent use dicalcium phosphate dihydrate, also can suppress the particle Chemical bond each other of dicalcium phosphate dihydrate.
In the above-mentioned reagent owing to make dicalcium phosphate dihydrate (A) be carried on particle (B), thereby be difficult for dispersing, also excellence of the property handled.
For the above reasons, by using above-mentioned reagent, can reduce the particle diameter of dicalcium phosphate dihydrate (A) and can not reduce water-permeable.Therefore, but efficient is removed the fluorine in the draining well, as a result of, can reduce the fluorine concentration of handling in the water for a long time.Further, can be easy and high-recovery ground the reagent after using is reclaimed.
In the above-mentioned reagent, with respect to particle (B) 100 mass parts, preferably phosphoric acid hydrogen calcium dihydrate (A) is 1 mass parts～100 mass parts.By being set at above-mentioned scope, can make dicalcium phosphate dihydrate (A) efficient well by particle (B) load, can be made into water-permeable, reagent that removing property of fluorine is more excellent.With respect to particle (B) 100 mass parts, dicalcium phosphate dihydrate (A) is 5 mass parts～50 mass parts, 7 mass parts～15 mass parts more preferably more preferably.
Dicalcium phosphate dihydrate (A) is preferably powder, more preferably its median size is 10 μ m～100 μ m.By being the median size of above-mentioned scope, can make dicalcium phosphate dihydrate (A) effectively by particle (B) load, can be made into the reagent of removing property of fluorine excellence simultaneously.
The median size of above-mentioned dicalcium phosphate dihydrate (A) can be used the Microtrack 9320HRA of Nikkiso Company Limited's manufacturing by the random method of laser diffraction and scattering method (レ ー ザ ー Hui Zhe Wrong) measure.
About dicalcium phosphate dihydrate (A), particle surface also is one of optimal way by the mode of sensitization.If in water, to the processing that suspends of the powdery granule of dicalcium phosphate dihydrate (A), make this granule surface activityization, then will handle the fluorine immobilization in the object water and thawless effect further increases.
Particle (B) but be the particle of load dicalcium phosphate dihydrate (A).By making dicalcium phosphate dihydrate (A) by particle (B) load (load is held), can be made into the reagent of water-permeable, removing property of fluorine excellence.
As particle (B), can enumerate for example be generally used for that water purifies cross filter sand, filter rubble etc., but be not limited to these among the present invention.As particle (B), preferably use sand.
The effective diameter of particle (B) is preferably 0.3mm～3.0mm.Effective diameter is 0.4mm～1.0mm, 0.5mm～0.6mm more preferably more preferably.Be above-mentioned scope by making effective diameter, can make the water-permeable of reagent and removing property of fluorine more excellent.
Above-mentioned effective diameter is the particle diameter suitable with following size, and this is of a size of particle (B) is sieved the size of mesh that the 10 quality % that make total mass pass through.Specifically, use the standard network cribellum (size of JIS Z8801, nominal size: 0.3mm～3.0mm, cribellum:
The degree of depth: 45mm) carry out the rider separating tests, the particle diameter that its size of mesh of passing through for 10 quality % with total mass is suitable.
Above-mentioned particle (B) preferable particle size is essentially the particle of 0.3mm～3.0mm, is that the particle of 0.3mm～3.0mm forms by particle diameter in fact only more preferably.That is, as particle (B), the particle in whole particles (B) more than the preferred 90 quality % has the particle diameter of 0.3mm～3.0mm, and more preferably more than the 99 quality %, further preferred ratio is more than the 99.9 quality % to this ratio.Particle (B) especially preferably do not contain particle diameter less than the particle of 0.3mm, do not contain the particle that particle diameter surpasses 3.0mm.Be above-mentioned scope by making particle diameter, dicalcium phosphate dihydrate (A) can be made the more excellent reagent of removing property of water-permeable, fluorochemicals by useful load.Particle (B) does not most preferably contain the particle that particle diameter surpasses 2.8mm in fact, namely most preferably all in the particles (B) the above particle of 90 quality % do not have particle diameter above 2.8mm.
The particle diameter of above-mentioned particle (B) can by use the standard network cribellum (size of JIS Z8801, nominal size: 0.3mm～3.0mm, cribellum:
The degree of depth: 45mm) carry out the rider separating tests and try to achieve.For example, in that it is not contained under the situation of particle diameter above the particle of 2.8mm, use nominal size to be the cribellum of 2.8mm.
The preferred uniformity ratio of above-mentioned particle (B) is below 1.5.Because uniformity ratio is above-mentioned scope, dicalcium phosphate dihydrate (A) can be by particle (B) useful load, can be made into the more reagent of excellence and removing property of fluorine excellence of water-permeable.
The uniformity ratio of above-mentioned particle (B) can be measured according to JWWAA103-1:2004.
In the above-mentioned reagent, in the scope of the object of the invention, can contain dicalcium phosphate dihydrate (A) and particle (B) composition in addition as required, but preferably phosphoric acid hydrogen calcium dihydrate (A) and particle (B) total account for more than the 99 quality %.
Above-mentioned reagent can be by mixing pulverous dicalcium phosphate dihydrate (A) to obtain with particle (B).
The manufacture method of reagent is not particularly limited, for example can make by the manufacture method that comprises following operation, described operation is for using oblique drum type gravity type boat davit mixing machine (Pour trunk type gravity type boat davit ミ キ サ ー) operation that dicalcium phosphate dihydrate (A) and particle (B) are mixed.
Tiltedly drum type gravity type boat davit mixing machine is the mixing machine that is equipped with in oblique drum mechanism for the mixing vessel that dicalcium phosphate dihydrate (A) and particle (B) are mixed, and gets final product so long as be commonly referred to as the utensil of oblique drum type gravity type boat davit mixing machine.Tiltedly drum mechanism is for being used for making the mechanism of above-mentioned mixing vessel inclination.
Form as oblique drum type gravity type boat davit mixing machine, can enumerate and for example following mixing vessel is installed in the oblique bulging mechanism, and will be installed in the mixing machine etc. of the internal perisporium of this mixing vessel be used to the blade that mixes, described mixing vessel is that the frusto-conical container is integrated, make one open-ended, make the mixing vessel of other end obturation simultaneously.Above-mentioned mixing vessel preferably can be rotated.
When carrying out the mixing of above-mentioned dicalcium phosphate dihydrate (A) and particle (B), usually the peristome that makes oblique bulging mechanical operation and make tube (De ラ system) drops into dicalcium phosphate dihydrate (A) and particle (B) towards the top while mixing vessel is rotated in a certain direction.Utilize blade that input each material is kicked up and fall the below again, carry out this repeatedly and move to mix.
Tiltedly therefore drum type gravity type boat davit mixing machine can mix under the situation that dicalcium phosphate dihydrate (A) is well kept by the state of particle (B) load owing to can come according to the behavior of input material mixing is promoted.Therefore, in the manufacturing of above-mentioned reagent, given play to excellent especially effect.
As the manufacture method of above-mentioned reagent, preferably dicalcium phosphate dihydrate (A) and particle (B) are fed in the mixing vessel of oblique drum type gravity type boat davit mixing machine, add water as required and mix.
As the sand that holds in the reactive tank of the present invention, be preferably and handle the inert substance that object water does not react.And preferably satisfy following enumerate in the characteristic at least 1, more preferably satisfy the following all characteristics of enumerating.
(1) do not contain impurity such as rubbish, clay matter or flat or frangible partially sand etc. in a large number, and contain quartzose in a large number, firm evenly; (2) content of iron sand or frangible sand etc. is few; (3) cleaning turbidity (cleaning the Turbid degree) is below 30 degree; (4) relative density (density) is 2.57～2.67 (g/cm
3); (5) be below 0.75% scorching hot decrement (Strong Hot Minus amount); (6) rate of wear is below 3%; (7) content of iron and iron containing compounds is below 0.03 (mg/L); (8) manganese is below 0.005 (mg/L) with the content that contains manganic compound; (9) the hydrochloric acid soluble rate is below 3.5%.
The characteristic of above-mentioned sand can be that benchmark is measured according to Japanese water channel association criterion JWWAA103-1:2006.
First layer of sand is formed by first sand of effective diameter less than particle (B).Effective diameter by making first sand can prevent dispersing of reagent less than particle (B).Thus, can improve the organic efficiency of the reagent after the use.
As long as the effective diameter of first sand is just unqualified less than the effective diameter of particle (B), for example is preferably 0.3mm～1.0mm, 0.3mm～0.6mm more preferably.
The first sand preferable particle size is essentially the particle of 0.3mm～0.6mm, is that the particle of 0.3mm～0.6mm forms by particle diameter in fact only more preferably.That is, as first sand, in whole first sand, the above particle of preferred 90 quality % has the particle diameter of 0.3mm～0.6mm, and the more preferably ratio with size particles of 0.3mm～0.6mm is that 95 quality % are above, further preferred ratio is more than the 99 quality %.First sand especially preferably do not contain particle diameter less than the particle of 0.3mm, do not contain the particle that particle diameter surpasses 0.6mm.Be above-mentioned scope by making particle diameter, can more effectively prevent dispersing of reagent.
The uniformity ratio of first sand is preferably below 1.5.Be above-mentioned scope by making uniformity ratio, can more effectively prevent dispersing of reagent.
Need to prove that the effective diameter of first sand, particle diameter and uniformity ratio can utilize the method identical with particle (B) to measure.
In first layer of sand, in the scope of the object of the invention, can contain first sand composition in addition as required, but preferred first sand total accounts for more than the 90 quality %.
The thickness of first layer of sand is not particularly limited, and is set at usually less than the reagent layer.Aspect consideration from preventing that effectively reagent from dispersing is preferably more than the 1cm.The upper limit of thickness is not particularly limited, and from being considered by the aspect that reclaims the reagent after using the reactive tank easily, is preferably below the 10cm.
Second layer of sand is made up of less than second sand of above-mentioned particle (B) effective diameter.Effective diameter by making second sand is less than particle (B), and the reagent that can suppress to constitute the reagent layer flows out, can improve the organic efficiency of the reagent after the use from reactive tank.
As long as the effective diameter of second sand is just unqualified less than the effective diameter of particle (B), for example is preferably 0.3mm～1.0mm, 0.3mm～0.6mm more preferably.By being set at above-mentioned scope, the further outflow of inhibited reaction agent, can improve the organic efficiency of the reagent after the use.
The second sand preferable particle size is essentially the particle of 0.3mm～0.6mm, is that the particle of 0.3mm～0.6mm forms by particle diameter in fact only more preferably.That is, as second sand, in whole second sand, the above particle of preferred 90 quality % has the particle diameter of 0.3mm～0.6mm, and the size particles with 0.3mm～0.6mm more preferably ratio is that 95 quality % are above, further preferred ratio is more than the 99 quality %.Second sand especially preferably do not contain particle diameter less than the particle of 0.3mm, do not contain the particle that particle diameter surpasses 0.6mm.Be above-mentioned scope by making particle diameter, the further outflow of inhibited reaction agent, can improve the organic efficiency of the reagent after the use.
The uniformity ratio of second sand is preferably below 1.5.Be above-mentioned scope by making uniformity ratio, the further outflow of inhibited reaction agent, can improve the organic efficiency of the reagent after the use.
Need to prove Department numbers such as the effective diameter of second sand, particle diameter and uniformity ratio (Jun) can utilize the method identical with particle (B) to measure.
In second layer of sand, in the scope of the object of the invention, can contain second sand composition in addition as required, but preferred second sand total accounts for more than the 90 quality %.
The thickness of second layer of sand is not particularly limited, and is set at usually less than the reagent layer.Consider from the aspect of the outflow that effectively prevents reagent, be preferably more than the 5cm.The upper limit of thickness is not particularly limited, and from being considered by the aspect that reclaims the reagent after using the reactive tank easily, is preferably below the 30cm.
Reactive tank of the present invention can prevent the outflow of reagent by having above-mentioned formation, as a result of, can improve the organic efficiency of the reagent after the use.
Reactive tank of the present invention preferably further has the 3rd layer of sand, and more preferably the 3rd layer of sand is arranged under second layer of sand.And the 3rd layer of sand preferably is made up of greater than the 3rd sand of second sand effective diameter.Because the effective diameter of the 3rd sand greater than second sand, can suppress to constitute the outflow of second sand of second layer of sand, but and then the outflow of inhibited reaction agent.Thus, can further improve the organic efficiency of the reagent after the use.
The effective diameter of the 3rd sand is preferably greater than the effective diameter of second sand, is not particularly limited as its scope, for example is preferably 0.5mm～3.0mm, 0.6mm～1.0mm more preferably.By being set at above-mentioned scope, the further outflow of inhibited reaction agent, can improve the organic efficiency of the reagent after the use.
The 3rd sand preferable particle size is essentially the particle of 0.5mm～3.0mm, is that the particle of 0.5mm～3.0mm forms by particle diameter in fact only more preferably.That is, as the 3rd sand, in whole the 3rd sand, the above particle of preferred 90 quality % has the particle diameter of 0.5mm～3.0mm, and the size particles with 0.5mm～3.0mm more preferably ratio is that 95 quality % are above, further preferred ratio is more than the 99 quality %.The 3rd sand especially preferably do not contain particle diameter less than the particle of 0.5mm, do not contain particle diameter greater than the particle of 3.0mm.Be above-mentioned scope by making particle diameter, the further outflow of inhibited reaction agent, can improve the organic efficiency of the reagent after the use.
The uniformity ratio of the 3rd sand is preferably below 1.5.Be above-mentioned scope by making uniformity ratio, the further outflow of inhibited reaction agent, can improve the organic efficiency of the reagent after the use.
Need to prove that the effective diameter of the 3rd sand, particle diameter and uniformity ratio can utilize the method identical with particle (B) to measure.
In the 3rd layer of sand, in the scope of the object of the invention, can contain the 3rd sand composition in addition as required, but preferred the 3rd sand total accounts for more than the 90 quality %.
The thickness of the 3rd layer of sand is not particularly limited, and is preferably set to less than the reagent layer.Consider from the aspect of the outflow that effectively prevents reagent, be preferably more than the 5cm.The upper limit of thickness is not particularly limited, and from being considered by the aspect that reclaims the reagent after using the reactive tank easily, is preferably below the 50cm.
Reactive tank of the present invention preferably further accommodates rubble (sand profit), more preferably will be located under second layer of sand by above-mentioned gravelly metalling, perhaps has under the situation of the 3rd layer of sand at reactive tank of the present invention, more preferably it is located under the 3rd layer of sand.Because lamination has above-mentioned metalling, can suppress to constitute the outflow of second sand of second layer of sand, perhaps contain under the situation of the 3rd layer of sand at reactive tank of the present invention, can suppress to constitute the outflow of the 3rd sand of the 3rd layer of sand, but and then the inhibited reaction agent from reactive tank, flow out.The particle diameter of rubble is preferably greater than second sand, perhaps has under the situation of the 3rd layer of sand at reactive tank of the present invention, is preferably greater than the 3rd sand.
Metalling is that the rubble of 2mm～50mm forms by granularity preferably.By having the metalling of above-mentioned granularity, can further suppress to constitute the outflow of second sand of second layer of sand, perhaps have under the situation of the 3rd layer of sand at reactive tank of the present invention, can further suppress to constitute the outflow of the 3rd sand of the 3rd layer of sand, but and then the inhibited reaction agent from reactive tank, flow out.Thus, can further improve the organic efficiency of reagent.Consider that from the aspect of the organic efficiency of further raising reagent the granularity of rubble is preferably 2mm～20mm, 2mm～12mm more preferably.
The granularity of rubble can be that benchmark is measured according to Japanese water channel association criterion JWWAA103-4:2006.
As the rubble that is contained in the reactive tank of the present invention, be preferably and handle the inert substance that object water does not react.And preferably satisfy following enumerate in the characteristic at least 1, more preferably satisfy the rubble of the following all characteristics of enumerating.
(1) do not contain impurity such as rubbish, clay matter or flat or frangible partially particle etc. in a large number, have firm circle; (2) cleaning turbidity is below 30 degree; (3) major axis accounts for below the 2 weight % of whole gravel particles for the gravel particle of minor axis more than 5 times; (4) relative density under the surface drying state of saturation is 2.50 (g/cm
3) more than; (5) the hydrochloric acid soluble rate is below 3.5%.
The characteristic of above-mentioned rubble can be that benchmark is measured according to Japanese water channel association criterion JWWAA103-4:2006.
In the granularity of above-mentioned rubble % be preferably more than 85%, more preferably more than 95%.Because rubble has % in the above-mentioned granularity, can further suppress to constitute the outflow of second sand from reactive tank of second layer of sand, perhaps have under the situation of the 3rd layer of sand at reactive tank of the present invention, can further suppress to constitute the outflow of the 3rd sand from reactive tank of the 3rd layer of sand, further, can the inhibited reaction agent from reactive tank, flow out.Thus, can further improve the organic efficiency of reagent.
% in the granularity of rubble (% (Content (%)) in the granularity) can be that benchmark is measured according to Japanese water channel association criterion JWWA A103-4:2006.
The thickness of metalling is not particularly limited, and is preferably set to less than the reagent layer.Consider from the aspect of the outflow that effectively prevents reagent, be preferably more than the 5cm.The upper limit of thickness is not particularly limited, and from being considered by the aspect that reclaims the reagent after using the reactive tank easily, is preferably below the 30cm.
Then the treatment facility of the present invention that possesses above-mentioned reactive tank is described in detail.Treatment facility of the present invention is owing to possess above-mentioned reactive tank, thereby the reagent after can fully being removed the processing water behind the fluorine easy and economically and can reclaiming use expeditiously.
Treatment facility of the present invention possesses: be used for storing the processing object water retention basin of handling object water; Above-mentioned reactive tank; Be used for handling object water by processing object water retention basin be supplied to reactive tank pipe arrangement; And be used for handling the pipe arrangement that water is discharged from reactive tank, this processing water make processing object water in reactive tank by obtaining.
Handle object water retention basin for being used for storing the groove of handling object water.The processing object water that stores in handling object water retention basin is supplied in the reactive tank by pipe arrangement.The volume of processing object water retention basin, the degree of depth, material etc. are not particularly limited, and suitably set according to the amount of handling object water, the fluorine concentration of handling object water, the scale for the treatment of facility etc. to get final product.
To handle object water by handling the pipe arrangement that object water retention basin is supplied to reactive tank for being used for, as long as can supply with to reactive tank by handling object water retention basin handling object water, its form just is not particularly limited, it can be connected with reactive tank handling object water retention basin, can directly not contact with reactive tank yet, and an end of pipe arrangement is arranged on the top of the reactive tank of upper opening, will handle the object water supply to reactive tank by the there.And, also can have for delivery of the pump of handling object water midway etc. at pipe arrangement.
For reactive tank, as long as have the formation of reactive tank of the present invention, its mode is not particularly limited; As treatment facility of the present invention, for example, can make the mode of used treatment facility (Fig. 3) in the example 1 as described later, the equipment of being discharged by pipe arrangement for the processing water that makes the metalling that has passed through reactive tank; The also mode for the treatment of facility (Fig. 1) as described later is for the processing water of the metalling that will not pass through reactive tank is immediately discharged equipment at least 1 zone that stores for the time being in reactive tank by pipe arrangement.
Be used for to handle the pipe arrangement that water discharged by reactive tank and be generally used for and handle the outside discharge of water to treatment facility, but its mode is not particularly limited.For example, valve of the flow of draining being regulated can having of pipe arrangement midway etc. also can hold storage at the pipe arrangement of backwash water retention basin being connected to for handling water of pipe arrangement midway as described later.And can possess for handling pump that water carries as backwash water etc.
Accompanying drawing being shown herein, further is elaborated to an example for the treatment of facility of the present invention.
The sketch chart that schematically shows an example of the treatment facility that possesses reactive tank of the present invention is Fig. 1.
In treatment facility shown in Figure 1, handle object water and pass through pipe arrangement 18 by handling in the object water retention basin 21 via pump 22, be supplied to the reactive tank 10 of upper opening.At this moment, pipe arrangement does not directly contact with reactive tank, and an end of pipe arrangement is arranged on the top of the reactive tank of upper opening, is supplied with in the reactive tank by the there and handles object water.The processing object water that is supplied in the reactive tank passes first layer of sand, reagent layer, second layer of sand, metalling successively, fully removes fluorine, makes processing water.Resulting processing water is not discharged to outside the reactive tank immediately, and stores in first area 16.Along with handling the carrying out that object water is supplied with in the reactive tank, the water level in the first area rises., make the height of partition wall 32 be lower than the height of partition wall 31 herein, partition wall 32 is separated first area and second area 17, and partition wall 31 is opened first area and the region separation that is provided with reagent layer etc.When the first area is full water, when processing water overflows, handle water and flow in the second area.Thus, the processing water of second area is by discharging in the pipe arrangement 19.The flow of the processing water of discharging is regulated by valve 33.Need to prove, when the processing water that is overflowed by the first area is transferred in the second area, handling water has crossed first area and the separated partition wall 32 of second area, inequality can not occur for the current that make the processing water of crossing partition wall 32 evenly flow, can leave V breach 34 on the top of partition wall 32.Wherein, leave on the top of partition wall 32 under the situation of V breach 34, the height that also need be lower than partition wall 31 according to the height of partition wall 32 arranges.
Be such formation by making treatment facility, can make and pass through the processing water behind the metalling and store for the time being at first area and second area, and to being regulated by the output of the processing water of discharging in the reactive tank, thereby can fully prolong the duration of contact of handling object water and reagent layer.And can carry out extensiveization of equipment.
So, treatment facility of the present invention further has at least 1 to store the zone of handling water also is one of optimal way in reactive tank.
Treatment facility of the present invention further possesses: the backwash water retention basin that is used for storing backwash water; Be used for the processing water supply that to discharge from the reactive tank pipe arrangement to the backwash water retention basin; And be used for storing at the processing water supply of the backwash water retention basin pipe arrangement to the reactive tank, the treatment facility of the present invention that further possesses above-mentioned part also is one of optimal way.
By having above-mentioned formation, treatment facility of the present invention can carry out recycling, use as backwash water resulting processing water.Thus, can reduce the output of handling water.Further, owing to resulting processing water can be used as backwash water, but thereby also cutting down cost.
The backwash water retention basin is for being used for storing the groove of backwash water, and its mode is not particularly limited, and the volume of backwash water retention basin, the degree of depth, material etc. can wait suitably according to the scale of the scale of the consumption of backwash water, reactive tank, treatment facility and set.
Being used for the processing water supply that will discharge from reactive tank for example will handle the pipe arrangement that water discharges from reactive tank with above-mentioned being used for to the pipe arrangement of backwash water retention basin and be connected.Its mode is not particularly limited, and amount, the formation of backwash water retention basin, the scale that can consider to handle water wait suitably and set.For example, can be at pipe arrangement possess for delivery of the pump of handling water midway etc.
Treatment process of the present invention comprise make contain fluorine processing object water in above-mentioned reactive tank by removing the operation of the fluorine in this processing object water.
The processing object water that contains fluorine is passed through in above-mentioned reactive tank, handle object water thus and contact with reagent, the fluorine of handling in the object water is removed.For treatment process, can the processing water of discharging from reactive tank be passed through again in reactive tank by 1 time in above-mentioned reactive tank, also namely can be by more than 2 times in above-mentioned reactive tank.
Treatment process of the present invention can comprise that to fluorine concentration be the operation that the processing water below the 0.8mg/L reclaims.Because water-permeable and the reaction efficiency excellence of above-mentioned reagent, but thereby efficient remove well that to handle the fluorine that contains in the object water, can make the fluorine concentration in the water be below the 0.8mg/L.
Treatment in accordance with the present invention method, the fluorine immobilization amount that can make every 1g dicalcium phosphate dihydrate (A) are more than the 1mg-F/g, are preferably more than the 10mg-F/g.
Treatment process of the present invention can be included in to handle adds calcium ion and generates Calcium Fluoride (Fluorspan) (CaF in the object water
2) the Calcium Fluoride (Fluorspan) that generates of operation and removing and fluorinion concentration reduced after the operation that reclaims of processing object water.These operations were preferably carried out before following operation: make contain fluorine processing object water in above-mentioned reactive tank by removing the operation of the fluorine in this processing object water.Because the lower calcium cpd of use cost in these operations, thereby particularly under the high situation of the fluorinion concentration of handling object water, can cutting down cost.Above-mentioned calcium ion is preferably with slaked lime (Ca (OH)
2), calcium carbonate (CaCO
3), calcium chloride (CaCl
2) wait the form of calcium cpd to add.
Resulting processing water be fluorine by the water after fully removing, fluorine concentration low (for example 0.8mg/L following) satisfies environmental protection standard.
The fluorine content of handling object water is not particularly limited, and no matter how few the or content of its content all can have been given play to excellent fluorine and remove ability, for example is preferably more than the 0.1mg/L.Consider that from the aspect of further having given play to effect of the present invention more preferably it surpasses 0.8mg/L.
Among the present invention, it is that the method for benchmark is measured that the fluorinion concentration in the fluorinated water can utilize with JIS K0102.
As handling object water, as long as for the water (fluorinated water) that contains fluorine just is not particularly limited, can enumerate the water in for example plant drainage, thermal water, rivers and creeks etc.As plant drainage, can enumerate the fluorine-containing draining of being discharged by silicon wafer manufacturing works, semiconductor fabrication factory etc.; Pickling draining by the discharge of metal factory; Aluminium surface treatment draining; Hydrofluoric acid is made draining; Fertilizer is made draining; Waste incineration draining etc.
Remove the aspect of efficient from the height that can obtain fluorion and consider that the pH that handles object water is preferably more than 3.Therefore, the processing water that is obtained by treatment process of the present invention (hereinafter also abbreviates " processing water " as.) pH also be preferably more than 3.More preferably above-mentioned pH is more than 4.The pH of above-mentioned processing object water or processing water can utilize sodium hydroxide, calcium hydroxide etc. that pH is adjusted to more than 3 less than pH is less than under 3 the situation under 3 the situation or in each operation.
In addition, the pH of above-mentioned processing object water and processing water is preferably below 11.If pH surpasses 11, then dicalcium phosphate dihydrate (A) may be difficult to carry out with the reaction of fluorion.Above-mentioned processing object water or the pH that handles water surpasses under 11 the situation or pH surpasses under 11 the situation in each operation can utilize hydrochloric acid etc. that pH is adjusted to below 11.
[embodiment]
Enumerate embodiment below and illustrate in greater detail the present invention, but the present invention is not limited to following examples.
(Production Example 1)
(Tohkemy makes with sand with high-rate fitration, " Japanese water channel association criterion JWWAA103-1:2004 standard prod, effective diameter: 0.6mm, uniformity ratio: below 1.5, maximum diameter 2.8mm is following, more than the path 0.3mm ") and the powder of dicalcium phosphate dihydrate (peaceful chemical industry manufacturing, " median size: 54 μ m " (DCPD hereinafter referred to as.)) be that 90 mass parts, DCPD are that the ratio of 10 mass parts is fed in the oblique drum type gravity type boat davit mixing machine (capacity 110L) according to the high-rate fitration sand in per 100 mass parts total amounts, carry out mixing in 3 minutes, obtain reagent.
(making example 1)
The reagent that obtains in the use Production Example 1 and sand and rubble as follows are made reactive tank.
First sand (high-rate fitration is made with sand (anxious fast Filter Over sand), Tohkemy, " Japanese water channel association criterion JWWAA103-1:2006 standard prod, effective diameter: 0.5mm, uniformity ratio: below 1.5, below the maximum diameter 2mm, more than the path 0.3mm ")
Second sand (high-rate fitration is made with sand, Tohkemy, " Japanese water channel association criterion JWWAA103-1:2006 standard prod, effective diameter: 0.5mm, uniformity ratio: 1.5 below, below the maximum diameter 2mm, more than the path 0.3mm ")
The 3rd sand (high-rate fitration is made with sand, Tohkemy, " Japanese water channel association criterion JWWAA103-1:2006 standard prod, effective diameter: 1mm, uniformity ratio: 1.5 below, below the maximum diameter 2.8mm, more than the path 0.5mm ")
Rubble (filter with rubble, Tohkemy and make, " in Japanese water channel association criterion JWWAA103-4:2006 standard prod, granularity: 4～8mm, the granularity more than the %:85% ")
As reactive tank, use volume to be 12cm, height acrylic (the ア Network リ Le) container made as 200cm as 22.6L, internal diameter.This reactive tank possess for will handle the object water supply to the reactive tank pipe arrangement and be used for handling the pipe arrangement that water (this processing water makes processing object water obtain by reactive tank) is discharged from reactive tank.
In above-mentioned reactive tank, drop into rubble (1kg), the 3rd sand (2kg), second sand (1kg) reagent (5kg) and first sand (0.5kg) successively, obtain reactive tank shown in Figure 2.In reactive tank 10, be provided with first layer of sand 11 (2cm), reagent layer 12 (30cm), second layer of sand 13 (5cm), the 3rd layer of sand 14 (10cm) and metalling 15 (5cm) successively from top.
Use the treatment facility possess above-mentioned reactive tank below, describe for the treatment process of the processing object water that contains fluorine.
As shown in Figure 3, treatment facility possesses:
(1) stores the processing object water retention basin 21 of handling object water;
(2) reactive tank 10;
(3) be used for to handle the object water supply to the pipe arrangement 18 of reactive tank 10;
(4) be used for to handle the object water supply to the pump 22 of reactive tank 10;
(5) be used for to handle the pipe arrangement 19 that water is discharged from reactive tank 10, thereby this processings water is processing object water by the fluorine in reactive tank 10, the processing object water and the reagent in the reactive tank 10 to react and makes the processing water of removing behind the fluorine;
(6) the backwash water retention basin 24;
(7) for will handle water supply to backwash water retention basin 24 from pipe arrangement 19 pipe arrangements of telling 29;
(8) be supplied to the pipe arrangement 28 that is connected with pipe arrangement 19 in the reactive tank 10 for the backwash water (processing water) that will store in the backwash water retention basin;
(9) for the pump 23 that backwash water is supplied to reactive tank; And
(10) be used for the pipe arrangement 25 of water supplies such as tap water to backwash water retention basin 24.
Handling object water is supplied in the reactive tank 10 by pipe arrangement 18 by handling object water retention basin 21.The processing object water of supplying with from the top of reactive tank 10 successively by first layer of sand 11 in the reactive tank 10, reagent layer 12,
Second layer of sand 13, the 3rd layer of sand 14 and metalling 15.Handle the fluorine that contains in the object water and by reagent layer 12 time, react with reagent, the formation fluorapatite.Obtain handling the processing water that the fluorine in the object water is removed thus.
For the reagent after using is carried out efficient recovery, need prevent that reagent from flowing out from reactive tank 10.In the reactive tank 10 of making example 1, below reagent layer 12, possess second layer of sand 13, thereby can effectively prevent the outflow of reagent.Prevent that by further possessing the 3rd layer of sand 14 and metalling 15, can making the effect that reagent flows out from further being improved.
In addition, because above-mentioned reactive tank possesses first layer of sand, thereby the dispersing of reagent can prevent that handling water injects the time.
Above-mentioned reactive tank can effectively prevent dispersing, flowing out of reagent by having above-mentioned formation, as a result of, can the reagent after using be reclaimed easy and high organic efficiency ground.
Resulting processing water is discharged from pipe arrangement 19.Handling water can be discharged to outside the treatment facility by pipe arrangement 19, and part or all of processing water passed through pipe arrangement 29 and stored in backwash water retention basin 24, can be made into backwash water.Backwash water is supplied in the reactive tank 10 by pipe arrangement 28 when carrying out the cleaning of reactive tank 10, is used for the cleaning of reactive tank 10 etc.
In backwash water retention basin 24, water such as tap water can store wherein by pipe arrangement 25, also it can be used as backwash water.
Be used as backwash water by the processing water that will reclaim, can reduce the output of handling water.
(embodiment 1)
Dropping into the 500L fluorinion concentration in the processing object water retention basin 21 of making example 1 treatment facility is the processing object water of 3mg/L (S1), be set at 20 liters/hour with handling the speed (water flowing flow) that object water supplies with in the reactive tank 10, handle handling object water.The processing water (the processing water in the pipe arrangement 19) of discharging from reactive tank 10 is carried out the part sampling, and (S2) measures to its fluorinion concentration, and the result is 0.1mg/L.
The mensuration of fluorinion concentration is that benchmark carries out with JIS K0102.
(embodiment 2～8)
Except put into the amount of processing object water that the fluorinion concentration of handling in the object water retention basin 21 is 3mg/L (S1) by change shown in the table 1, handle similarly to Example 1, the fluorinion concentration (S2) of handling aftertreatment water is measured.Measurement result is listed in table 1.
[table 1]
[industrial applicibility]
Reactive tank of the present invention and treatment facility be owing to have an above-mentioned formation, thereby the field that can suitably be used for having the water that contains fluorine to generate.
[explanation of symbol]
10: reactive tank
11: the first layers of sand
12: the reagent layer
13: the second layers of sand
14: the three layers of sand
15: metalling
16: the first area
17: second area
18,19,25,28,29: pipe arrangement
21: handle object water retention basin
22,23: pump
24: the backwash water retention basin
31,32: partition wall
33: valve
The 34:V breach
Claims (11)
1. reactive tank, it is for being used for removing from the processing object water that contains fluorine the reactive tank of fluorine, and this reactive tank is characterised in that,
Accommodate sand and reagent in above-mentioned reactive tank, above-mentioned sand and above-mentioned reagent constitute first layer of sand, reagent layer and second layer of sand successively from the top of above-mentioned reactive tank;
Above-mentioned reagent contains dicalcium phosphate dihydrate (A) and particle (B), and dicalcium phosphate dihydrate (A) is by particle (B) load;
Above-mentioned first layer of sand is made up of less than first sand of above-mentioned particle (B) effective diameter;
Above-mentioned second layer of sand is made up of less than second sand of above-mentioned particle (B) effective diameter.
2. reactive tank as claimed in claim 1, wherein, this reactive tank further has the 3rd layer of sand, and above-mentioned the 3rd layer of sand is made up of greater than the 3rd sand of second sand effective diameter, and above-mentioned the 3rd layer of sand is located under second layer of sand.
3. reactive tank as claimed in claim 1, wherein, this reactive tank further accommodates rubble, is located under second layer of sand by the metalling that above-mentioned rubble is formed.
4. reactive tank as claimed in claim 2, wherein, this reactive tank further accommodates rubble, is located under the 3rd layer of sand by the metalling that above-mentioned rubble is formed.
5. as claim 1,2,3 or 4 described anti-grooves, wherein, particle (B) is that effective diameter is the particle of 0.3mm～3.0mm.
6. as claim 1,2,3,4 or 5 described reactive tanks, wherein, the uniformity ratio of particle (B) is below 1.5.
7. as claim 1,2,3,4,5 or 6 described reactive tanks, wherein, the median size of dicalcium phosphate dihydrate (A) is 10 μ m～100 μ m.
8. treatment facility, it is for being used for removing from the processing object water that contains fluorine the treatment facility of fluorine, and this treatment facility is characterised in that it possesses:
Be used for storing the processing object water retention basin of handling object water;
Claim 1,2,3,4,5,6 or 7 described reactive tanks;
Be used for above-mentioned processing object water by handling the pipe arrangement that object water retention basin is supplied to reactive tank; And
Be used for handling the pipe arrangement that water is discharged from reactive tank, this processing water make above-mentioned processing object water in reactive tank by obtaining.
9. treatment facility as claimed in claim 8 wherein, further has at least 1 and stores the zone of handling water in reactive tank.
10. treatment facility as claimed in claim 8 or 9, wherein, this treatment facility further possesses:
Be used for storing the backwash water retention basin of backwash water;
Be used for the processing water supply that to discharge from reactive tank to the pipe arrangement of backwash water retention basin; And
Be used for to store at the processing water supply of the backwash water retention basin pipe arrangement to the reactive tank.
11. a treatment process is characterized in that, this treatment process comprises following operation: make contain fluorine processing object water in claim 1,2,3,4,5,6 or 7 described reactive tanks by removing the fluorine in this processing object water.
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|---|---|---|---|
| JP2012-029337 | 2012-02-14 | ||
| JP2012029337 | 2012-02-14 |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105271496A (en) * | 2015-10-26 | 2016-01-27 | 苏州书瑞环保科技有限公司 | Environment-friendly nano sedimentation agent for water treatment and preparation method of sedimentation agent |
| TWI586606B (en) * | 2016-07-25 | 2017-06-11 | 中國鋼鐵股份有限公司 | Method of producing iron silicate powder |
| CN109250842A (en) * | 2018-10-09 | 2019-01-22 | 北京朗新明环保科技有限公司 | A kind of method and process system of fluorine-containing industrial waste water with high ammoniac nitrogen circular treatment |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106693877B (en) * | 2016-11-30 | 2019-04-23 | 江苏永冠给排水设备有限公司 | It is a kind of that connection formula runner reaction kettle equipment and its application method are adjoined based on planting method fluorine removal water process |
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|---|---|---|---|---|
| CN2748149Y (en) * | 2004-03-29 | 2005-12-28 | 安逢龙 | Upper flow type deep molding sand filter |
| CN1850640A (en) * | 2006-05-31 | 2006-10-25 | 同济大学 | Artificial reinforced land percolation sewage treatment apparatus |
| WO2010134573A1 (en) * | 2009-05-21 | 2010-11-25 | ダイキン工業株式会社 | Treatment agent and process for production thereof, and treatment method |
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- 2013-02-13 JP JP2013025631A patent/JP2013188740A/en active Pending
- 2013-02-16 CN CN2013100511623A patent/CN103241858A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN2748149Y (en) * | 2004-03-29 | 2005-12-28 | 安逢龙 | Upper flow type deep molding sand filter |
| CN1850640A (en) * | 2006-05-31 | 2006-10-25 | 同济大学 | Artificial reinforced land percolation sewage treatment apparatus |
| WO2010134573A1 (en) * | 2009-05-21 | 2010-11-25 | ダイキン工業株式会社 | Treatment agent and process for production thereof, and treatment method |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105271496A (en) * | 2015-10-26 | 2016-01-27 | 苏州书瑞环保科技有限公司 | Environment-friendly nano sedimentation agent for water treatment and preparation method of sedimentation agent |
| TWI586606B (en) * | 2016-07-25 | 2017-06-11 | 中國鋼鐵股份有限公司 | Method of producing iron silicate powder |
| CN109250842A (en) * | 2018-10-09 | 2019-01-22 | 北京朗新明环保科技有限公司 | A kind of method and process system of fluorine-containing industrial waste water with high ammoniac nitrogen circular treatment |
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Application publication date: 20130814 |