CN103896372B - Glow discharge associated treatment is utilized to contain As (III), the method for Cr (VI) waste water and device thereof - Google Patents
Glow discharge associated treatment is utilized to contain As (III), the method for Cr (VI) waste water and device thereof Download PDFInfo
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Abstract
The present invention relates to environment sewage treatment field, particularly one utilizes glow discharge associated treatment to contain As (III), the method for Cr (VI) waste water and device thereof.Plasma technique is applied to containing As? (III), Cr? (VI) system for handling of waste water, glow discharge system is utilized to work in coordination with, efficiently by As? (III), Cr? (VI) As that toxicity is less is converted into? (V), Cr? (III), the waste water effect of wherein a kind of objectionable impurities is contained relative to process, does the present invention process containing As simultaneously? (III), Cr? (VI) better effects if of the waste water of two kinds of materials, does not need any chemical reagent.And required equipment is simple, easy to operate, cost is also lower, is convenient to promote the use of.
Description
Technical field
The present invention relates to environment sewage treatment field, particularly one utilizes glow discharge associated treatment to contain As (III), the method for Cr (VI) waste water and device thereof.
Background technology
Along with developing rapidly of industrial technology, the objectionable impurities contained in waste water is of a great variety, except traditional organic contamination beyond the region of objective existence, also containing a large amount of poisonous mineral ions, and such as Cr (VI), As (III).Arsenide is while the production fields such as mining, smelting, glass manufacture, agricultural chemicals and wood preservative are used widely, cause a considerable amount of arsenic compound entered environment, and be present in water body, soil, plant, animal, marine organisms and human body with different shape by chemical process and bio-transformation effect, and form circulation between each arsenide.The arsenic of different shape and valence state, physico-chemical property is different, and toxicity is also different, and the toxicity as arsenus acid is 2.5-60 times of arsenic acid, and organoarsenium compound is larger than the toxicity of inorganic arsenic chemicals again.Arsenic is not the essential element of human body, and arseniasis also can be divided into acute and chronic two kinds.Acute arsenic poisoning: Report many because of eat polluted by arsenic food, drink water or wrongly take and cause containing arsenic agricultural chemicals.Arsenicalism mostly is environmental pollution and the release of natural arsenic, more general than acute arsenic poisoning: Report.Long-term absorption low dosage arsenic, just falls ill through the more than ten years even body accumulation of decades.Arseniasis main manifestations is nerve injury, produces peripheral nerve inflammation etc.EPA (USEPA) announces, from 2006, in tap water, the maximum concentration of the arsenic of legal permission will be reduced to 0.01mg/L from 0.05mg/L.In Drinking Water in China standard GB5749-85, the maximum permissible concentration of regulation arsenic is 0.05mg/L, and the limit value of politics and law department of Ministry of Health arsenic in the middle regulation water quality of " drinking water sanitary standard " (paper for approval) in 2006 is 0.01mg/L.
Chemical method, physico-chemical process and microbial method are mainly contained for the treatment process of arsenic in arsenic-containing waste water.Coagulation Method is a kind of method that removing arsenic in water is comparatively conventional, the adsorption arsenic-adsorbing that the method mainly utilizes coagulating agent powerful, then by filter or with filter membrane except the arsenic in anhydrating.Experimental result shows, molysite to the removal efficiency of arsenic apparently higher than aluminium salt.Molysite is most economical, the most effective precipitation agent.Equally, absorption method is a kind of simple wastewater processing technology, has efficient, easy and good selective, and particularly to lower concentration, contaminative by force, the arsenic-containing waste water that other method is difficult to effectively process has unique using value.But As (III) not only toxicity is large, and in ecotope, movability is strong, is difficult to be fixed.And the toxicity of As (V) is relatively little, and easily adsorbed, be able to efficient removal.In the experiment and actual application of Coagulation Method and absorption arsenic removal, it is found that the removal effect of As (V) apparently higher than As (III).So, in arsenic removal process, often preoxidation is carried out to handled waste water, namely As (III) initial oxidation is become As (V), and then remove.Conventional oxygenant mainly contains chlorinated lime, hydrogen peroxide, chlorine, ozone and Manganse Dioxide etc.But the method needs to add a large amount of precipitation agents, produce a large amount of arsenic-containing waste residues and also can cause secondary pollution, therefore make the application of the method be restricted.
Chromium is one of heavy metal common in environment, and seldom containing chromium in natural water body, the heavy metal chromium pollution of water body and soil is mainly from the random discharge of the production process chromate waste water such as mining, plating, metallurgy, dyestuff, process hides, wood preservation and waste residue.Chromium cpd mainly contains Cr (III) and Cr (VI) two kinds of existence forms in the environment, if be subject to the impact of the factors such as temperature in environment, pH value, organism, Cr (III) in water body and Cr (VI) can transform mutually, wherein the bio-toxicity of Cr (VI) is higher than Cr (III) toxicity 100 times, be one of internationally recognized 3 kinds of carcinogenic metal objects, in water, Cr (VI) content is greater than 0.5mg/L and will be detrimental to health.Cr (VI) easily moves in soil and the aqueous solution, and it invades human body by air, drinking-water, food or contact, causes skin erosion, respiratory tract infection, liver dysfunction even lung cancer.
At present, the method for administering both at home and abroad pollution of chromium is more, mainly contains method of chemical treatment, ion exchange method, electrolytic process, adsorption treatment method, liquid membrane separation method, biochemical process, first supercritical processing method, ion floatation method are several.But these method efficiency are comparatively slow or need to add a large amount of chemical reagent, and therefore cost is high, and easily causes secondary pollution.
Summary of the invention
The present invention is directed to deficiency of the prior art, provide one to utilize glow discharge associated treatment to contain As (III), the method for Cr (VI) waste water and device thereof.
A kind of plasma technique is applied to the system for handling containing As (III), Cr (VI) waste water, glow discharge system is utilized to work in coordination with, efficiently As (III), Cr (VI) are converted into the less As of toxicity (V), Cr (III), relative to the waste water effect of process containing a kind of objectionable impurities, the present invention processes the better effects if of the waste water containing As (III), Cr (VI) simultaneously.
Technical scheme of the present invention is:
One utilizes glow discharge associated treatment to contain the method for As (III), Cr (VI) waste water: comprise the following steps:
(1) pending is imported to electrode glow discharge water treatment device containing Cr (VI), As (III) waste water solution adjust ph and conductivity value;
(2) under atmospheric atmosphere or rare gas element, carry out glow discharge, connect direct supply and carry out discharge process; After discharge process, Cr (VI) reduction in solution, As (III) oxidation, realize the process to poisonous ion.
On the basis of above scheme, will be adjusted to 2-7 containing Cr (VI), As (III) waste water solution pH value in described step (1), specific conductivity adjusts to 4-7mS/cm.
For the adjustment of pH in described step (1), different pH can be selected according to the concentration of two kinds of harmful ions, processing requirements, the more little process being more conducive to Cr (VI) of pH value, pH value is more conducive to more greatly the process of As (III).
On the basis of above scheme, stir in discharge process process in described step (2), stir speed (S.S.) is that 2-3 turns/s, and the discharge process time is 10-20 minute.
On the basis of above scheme, the voltage of the direct supply in described step (2) is 480-1000V, and electric current is 80-500mA.
The invention also discloses the electrode glow discharge water treatment device adopted in a kind of aforesaid method, comprise carbon-point negative electrode, stainless steel needle-like anode, glass reactor, Glass tubing, described carbon-point negative electrode and Glass tubing are separately positioned on described glass reactor and cover; Described glass reactor periphery arranges cold hydrazine interlayer, described cold hydrazine interlayer is arranged cooling water inlet and cooling water outlet mouth; The bottom of described Glass tubing seals with quartzy core, and described carbon-point negative electrode is placed in described Glass tubing.
On the basis of above scheme, the quantity of described stainless steel needle-like anode is 1-6 root.
On the basis of above scheme, stirring magneton is set in described glass reactor.
In contact glow discharge electrolysis process, the generation of plasma body is as follows: high-voltage DC power supply is added to the two poles of the earth of glass reactor, electrolysis occurs, between electrode, produces high current.Due to the effect of joule heating, the solvent rapid vaporization around stainless steel needle-like anode, resistance increases sharply, because the resistance of now electrolytic solution obvious change does not occur, so voltage is almost all added on the gas around stainless steel needle-like anode.Because the radius-of-curvature of stainless steel needle-like anode is very little, thus produce glow discharge plasma.
The invention has the beneficial effects as follows:
(1) glow discharge electrolysis plasma body belongs to nonequilibrium plasma, is a kind of electrochemical method of novel generation plasma body.The most significant feature of glow discharge electrolysis is non-faraday's property, can produce the materials such as a large amount of hydroxyl radical free radicals and hydrogen peroxide, produce the UV-light of wide wavelength simultaneously in discharge process.Wherein Cr (VI) effectively can be converted into Cr (III) by the reducing substances such as hydrated electron, hydrogen atom and hydrogen peroxide, and As (III) effectively can be oxidized to As (V) by the hydroxyl radical free radical generated.In glow discharging process, chromium ion transform process product can by hydrogen peroxide converting be hydroxyl radical free radical, the oxidation of As (III) can be promoted.In addition, the existence due to As (III) consumes the hydroxyl radical free radical that part produces, and the Cr (III) decreasing generation is oxidized to the probability of Cr (VI) again.Therefore, in the treating processes be used for containing the two ion waste water solution in glow discharge, the two ion can be mutually promoted respective processing efficiency, and therefore total treatment effect is obtained for raising.
(2) the present invention utilizes glow discharge device to process containing As (III), Cr (VI) waste water simultaneously, and method is unique novel, and processing efficiency is high, does not need any chemical reagent.And required equipment is simple, easy to operate, cost is also lower, is convenient to promote the use of.
(3) device electrical discharge zone of the present invention is comparatively large, to the reduction rate of Cr (VI) and the oxidation rate of As (III) fast, efficiency is high, greenization.When processing this two kinds of objectionable impuritiess, both treatment effects are better than the effect of a kind of objectionable impurities of independent processing simultaneously.
(4) under other metal ions of existence or organic disturbed condition, still higher processing efficiency can be kept.
Accompanying drawing explanation
Accompanying drawing 1 is the structural representation of electrode glow discharge device of the present invention;
Accompanying drawing 2 is the vertical view of electrode glow discharge device of the present invention;
Accompanying drawing 3 is the oxidation efficiency of As (III) and the reduction efficiency of Cr (VI) when processing the waste water containing As (III), Cr (VI)
Wherein, a in () (b) (c), filled box processes the oxidation efficiency simultaneously containing As (III) when As (III), Cr (VI) waste water, open squares is the oxidation efficiency of process only containing As (III) during As (III) waste water;
D in () (e) (f), solid rim processes the reduction efficiency simultaneously containing Cr (VI) when As (III), Cr (VI) waste water, open circle is the reduction efficiency of process only containing Cr (VI) during Cr (VI) waste water;
Accompanying drawing 4 is the impact on the oxidation efficiency of As (III) and the reduction efficiency of Cr (VI) when containing organism in waste water
Wherein, a () filled box is the oxidation efficiency of As (III) when processing As (III), Cr (VI) the composite waste solution not containing ethanol, open squares is the oxidation efficiency of As (III) when processing As (III), Cr (VI) the composite waste solution containing 0.5mM ethanol; B () solid rim is the reduction efficiency of Cr (VI) when processing As (III), Cr (VI) the composite waste solution not containing ethanol, open circle is the reduction efficiency of Cr (VI) when processing As (III), Cr (VI) the composite waste solution containing 0.5mM ethanol;
Accompanying drawing 5 is the impact on the oxidation efficiency of As (III) and the reduction efficiency of Cr (VI) when containing different metal ion in waste water
Wherein, the oxidation efficiency of (a) process containing As (III) during As (III), Cr (VI) the composite waste solution of different metal ion; The reduction efficiency of (b) process containing Cr (VI) during As (III), Cr (VI) the composite waste solution of different metal ion.
Embodiment
The specific embodiment of the present invention is as follows:
Embodiment 1:
Utilize the efficient Quick Oxidation of glow discharge to fix a treatment process for arsenic in waste water, comprise the following steps:
(1) by pending containing Cr (VI), As (III) waste water solution adjust ph be 2 and conductivity value 7mS/cm import to electrode glow discharge water treatment device;
(2) glow discharge reactor described in as shown in Figure 1, applying 4 pin electrodes is stainless steel needle-like anode 2, negative electrode is carbon electrode 1, and it is isolated with solution by the Glass tubing 4 of sealed bottom core, when discharging, every root pin electrode contacts with liquid level, and under atmospheric atmosphere or rare gas element, carry out glow discharge, normal operation DC voltage is 480V, electric current is 80mA, and stir speed (S.S.) is 2 turns/s; After discharge process, Cr (VI) reduction in solution, As (III) oxidation, realize the process to poisonous ion.
Embodiment 2:
Utilize the efficient Quick Oxidation of glow discharge to fix a treatment process for arsenic in waste water, comprise the following steps:
(1) by pending be 5 and conductivity value 4mS/cm containing As (III) waste water solution adjust ph, import to electrode glow discharge water treatment device;
(2) it is stainless steel needle-like anode that the glow discharge reactor described in applies 2 pin electrodes, negative electrode is carbon electrode, and by the Glass tubing of sealed bottom core and solution isolated, when discharging, every root pin electrode contacts with liquid level, glow discharge is carried out under atmospheric atmosphere or rare gas element, normal operation DC voltage is 1000V, and electric current is 500mA, and stir speed (S.S.) is 2 turns/s; After discharge process, Cr (VI) reduction in solution, As (III) oxidation, realize the process to poisonous ion.
Embodiment 3:
The processing efficiency to two kinds of materials relatively under condition of different pH, and the effect comparison a kind of with individual curing.
As Fig. 1, a kind of electrode glow discharge water treatment device, comprises carbon-point negative electrode 1, stainless steel needle-like anode 2, glass reactor 3, Glass tubing 4, and described carbon-point negative electrode 1 and Glass tubing 4 are separately positioned on described glass reactor 3 and cover; Described glass reactor 3 periphery arranges cold hydrazine interlayer 6, described cold hydrazine interlayer 6 is arranged respectively cooling water inlet 7 and cooling water outlet mouth 8; The bottom of described Glass tubing 4 seals with quartzy core, and described carbon-point negative electrode 1 is placed in described Glass tubing 4.
Allocate three kinds of pending solution:
(1) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is respectively 2,3 and 5;
(2) Cr (VI) concentration is the solution 150mL of 31mg/L, and pH value is respectively 2,3 and 5;
(3) As (III) concentration is the solution 150mL of 75mg/L, and pH value is respectively 2,3 and 5.
Utilize sodium sulfate that three kinds of electrical conductivity of solution are adjusted to 5mS/cm, inject glow discharge reactor respectively, be about 580V at voltage, electric current 120mA, discharge process 18 minutes under the condition of an employing pin electrode, every sampling in 3 minutes once.
Experimentally result, as shown in Figure 3, when pH is 2, the reduction effect of chromium is better.When pH is 5, the oxidation effectiveness of arsenic is better.And effect during the two combination treatment is higher than the effect of a kind of material of individual curing, see Fig. 3 (a) (b) (c) (d) (e) (f).As can be seen here, utilize glow discharge process contain Cr (VI), As (III) waste water time, two kinds of materials are to there being associated treatment effect each other.
Experimental example 4: compare waste water solution containing during organism on the impact of final treatment effect
As Fig. 1, a kind of electrode glow discharge water treatment device, comprises carbon-point negative electrode 1, stainless steel needle-like anode 2, glass reactor 3, Glass tubing 4, and described carbon-point negative electrode 1 and Glass tubing 4 are separately positioned on described glass reactor 3 and cover; Described glass reactor 3 periphery arranges cold hydrazine interlayer 6, described cold hydrazine interlayer 6 is arranged respectively cooling water inlet 7 and cooling water outlet mouth 8; The bottom of described Glass tubing 4 seals with quartzy core, and described carbon-point negative electrode 1 is placed in described Glass tubing 4.
Allocate two kinds of pending solution:
(1) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3;
(2) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3, and alcohol concn is 0.5mM.
Utilize sodium sulfate that three kinds of electrical conductivity of solution are adjusted to 5mS/cm, inject glow discharge reactor respectively, be about 580V at voltage, electric current 120mA, discharge process 18 minutes under the condition of an employing pin electrode, every sampling in 3 minutes once.
Experimentally result, as shown in Figure 4, when 0.5mM ethanol organism exists, the oxidation efficiency of As (III) reduces slightly, and the reduction efficiency of Cr (VI) increases slightly.
Embodiment 5: compare the impact of waste water solution when containing other metal ions on final treatment effect
As Fig. 1, a kind of electrode glow discharge water treatment device, comprises carbon-point negative electrode 1, stainless steel needle-like anode 2, glass reactor 3, Glass tubing 4, and described carbon-point negative electrode 1 and Glass tubing 4 are separately positioned on described glass reactor 3 and cover; Described glass reactor 3 periphery arranges cold hydrazine interlayer 6, described cold hydrazine interlayer 6 is arranged respectively cooling water inlet 7 and cooling water outlet mouth 8; The bottom of described Glass tubing 4 seals with quartzy core, and described carbon-point negative electrode 1 is placed in described Glass tubing 4.
Allocate five kinds of pending solution:
(1) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3;
(2) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3, Co
2+concentration is 0.5mM;
(3) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3, Ni
2+concentration is 0.5mM;
(4) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3, Cu
2+concentration is 0.5mM;
(5) the mixing solutions 150mL of Cr (VI) concentration to be 31mg/L, As (III) concentration be 75mg/L, pH value is 3, Mn
2+concentration is 0.5mM.
Utilize sodium sulfate that three kinds of electrical conductivity of solution are adjusted to 5mS/cm, inject glow discharge reactor respectively, be about 580V at voltage, electric current 120mA, discharge process 18 minutes under the condition of an employing pin electrode, every sampling in 3 minutes once.
Experimentally result, as shown in Fig. 5 (a) (b), when 0.5mM different metal ion exists, Cu
2+, Ni
2+, Co
2+and Mn
2+little on the oxidation impact of As (III).When 0.5mM different metal ion exists, Ni
2+, Cu
2+and Mn
2+the reduction of Cr (VI) can be promoted, Co
2+slightly can contain the reduction of Cr (VI).
Claims (5)
1. utilize glow discharge associated treatment to contain a method for As (III), Cr (VI) waste water, it is characterized in that: comprise the following steps:
(1) pending is imported to electrode glow discharge water treatment device containing Cr (VI), As (III) waste water solution adjust ph and conductivity value, described pH value is adjusted to 2-7, and described specific conductivity adjusts to 4-7mS/cm;
(2) under atmospheric atmosphere or rare gas element, carry out glow discharge, connect direct supply, the voltage of direct supply is 480-1000V, and electric current is that 80-500mA carries out discharge process; After discharge process, Cr (VI) reduction in solution, As (III) oxidation, realize the process to poisonous ion.
2. the method utilizing glow discharge associated treatment to contain As (III), Cr (VI) waste water according to claim 1, it is characterized in that, stir in discharge process process in described step (2), stir speed (S.S.) is that 2-3 turns/s, and the discharge process time is 10-20 minute.
3. one kind according to the electrode glow discharge water treatment device described in claim 1, it is characterized in that: comprise carbon-point negative electrode (1), stainless steel anode (2), glass reactor (3), Glass tubing (4), described carbon-point negative electrode (1) and Glass tubing (4) are separately positioned on described glass reactor (3) and cover; Described glass reactor (3) periphery arranges cold hydrazine interlayer (6), described cold hydrazine interlayer (6) is arranged respectively cooling water inlet (7) and cooling water outlet mouth (8); The bottom of described Glass tubing (4) seals with quartzy core, and described carbon-point negative electrode (1) is placed in described Glass tubing (4).
4. electrode glow discharge water treatment device according to claim 3, is characterized in that the quantity of described stainless steel anode (2) is 1-6 root.
5. electrode glow discharge water treatment device according to claim 3, is characterized in that arranging in described glass reactor (3) and stirs magneton (9).
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| CN106040739A (en) * | 2016-08-08 | 2016-10-26 | 西北农林科技大学 | Device and method for remediation of trivalent arsenic contaminated sites |
| CN106744676A (en) * | 2017-01-23 | 2017-05-31 | 上海朗研光电科技有限公司 | The device and its synthetic method of glow discharge synthesizing nano-particle |
| CN109507170B (en) * | 2018-12-06 | 2021-01-19 | 西北师范大学 | Miniaturized electrolyte contact glow discharge emission spectrum device |
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