CN101343102A - Adsorption and magnetic separation coupling method for recycling precious metal ion in precious metal - Google Patents
Adsorption and magnetic separation coupling method for recycling precious metal ion in precious metal Download PDFInfo
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- CN101343102A CN101343102A CNA2008100541308A CN200810054130A CN101343102A CN 101343102 A CN101343102 A CN 101343102A CN A2008100541308 A CNA2008100541308 A CN A2008100541308A CN 200810054130 A CN200810054130 A CN 200810054130A CN 101343102 A CN101343102 A CN 101343102A
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Abstract
The invention discloses an adsorption and magnetic separation coupling method for recovering noble metal ions in wastewater, comprising the steps of: firstly, selecting and adsorbing noble metal ions in a solution by magnetotactic bacteria in an adsorber; secondly, separating out the magnetotactic bacteria after adsorbing the metal ions from the mixture obtained in the first step by utilizing a magnetic separator; and thirdly, implementing the metal ion desorption treatment to the magnetotactic bacteria separated off from the second step and adsorbed with noble metal ions, and if an electrolytic method is adopted to carry out the further purification and recovery, the noble metal in wastewater can be finally acquired. The method utilizes the selective adsorption characteristic of magnetotactic bacteria and combines the high gradient magnetic separation technique to recover noble metal ions efficiently from liquid and purify the wastewater. The noble metal ions in the wastewater solution can be utilized and recovered effectively on the premise of ensuring high efficiency and environmental protection through implementing the technical proposal of the method.
Description
Technical field
The present invention relates to the technical field that precious metal ion reclaims, particularly relate to a kind of absorption and magnetic separation coupling method that reclaims precious metal ion in the waste water, this method has proposed absorption and has separated coupling technique with magnetic, utilized the selection characterization of adsorption of magnetotactic bacteria and in conjunction with the High-gradient Magnetic isolation technique, from solution, reclaimed precious metal ion efficiently and can purify liquid waste.
Background technology
Current, noble metal is widely used in industries such as Aeronautics and Astronautics, navigation, guided missile, rocket, nuclear power, microelectronics, chemical, inorganic materials, purifying air and metallurgy.Along with the fast development of national economy, the demand of noble metal is also being increased day by day.In the today that can utilize that noble metal is resource-constrained, resource supply and demand contradiction becomes increasingly conspicuous and environment constantly worsens, the recycling by waste is the basic place that solves the noble metal shortage problem.
According to statistics, only with regard to the household appliances product, China just has accumulative total to surpass 7.5 hundred million refrigerator, washing machine and televisor, 1,600 ten thousand computers of having an appointment in addition, and oneself faces renewal the major part in them.The printed circuit board (PCB) that is used in these electronic products, Gold Content per ton can reach about 300 grams, and copper content is also more considerable, therefore, deals carefully with above-mentioned " electronic waste ", turns waste into wealth, and have been subjected to the great attention of country, become the task of top priority.
At present both at home and abroad from waste reclaim precious metal the most frequently used be hydrometallurgic recovery technology (can be the patented technology scheme of US5304359 referring to U.S. Patent number), its great advantage is that facility investment is not high, the metal recovery rate height, but in the wet processing process, will produce waste gas, waste residue and waste liquid, and can cause secondary pollution.
In recent years, biosorption process receives much attention because of its potential application foreground in environment protection and precious metal recovery.Biosorption process is compared with the hydrometallurgic recovery technology, the low advantage of wide material sources, working cost with organic efficiency height, biological adsorption agent, but because the biological particles volume of free state is little, physical strength is low, be difficult to from solution, separate behind the absorption metal, make biological adsorption technology still rest on laboratory stage mostly.
Up to now, also there is not a kind of method guaranteeing effectively utilizing the precious metal ion that reclaims in the waste water solution under the prerequisite of efficient, environmental protection.
Summary of the invention
In view of this, the purpose of this invention is to provide a kind of absorption and magnetic separation coupling method that reclaims precious metal ion in the waste water, utilize magnetotactic bacteria absorption precious metal ion earlier, utilize high-gradient magnetic field that the magnetotactic bacteria behind the adsorbing metal ions is separated from mixed solution effectively then, can guarantee to effectively utilize the precious metal ion that reclaims in the waste water solution under the prerequisite of efficient, environmental protection.
For this reason, the invention provides a kind of absorption and magnetic separation coupling method that reclaims precious metal ion in the waste water, may further comprise the steps:
The first step, in adsorber, select precious metal ion in the adsorbent solution with magnetotactic bacteria;
Second goes on foot, utilizes the magnetotactic bacteria magnetic separator is isolated adsorbing metal ions from the mixed solution that the first step obtains after;
The 3rd step, the desorption that the isolated magnetotactic bacteria that is adsorbed with precious metal ion of second step is carried out metal ion are handled, if adopt electrolytic process to be further purified recovery, obtain the noble metal in the waste water the most at last.
Preferably, the described the first step is specially: contain the pH value of the solution of precious metal ion by adjusting, select precious metal ion in the adsorbent solution with magnetotactic bacteria in adsorber.
Preferably, described selection absorption Au
2+The appropriate pH value be 2.
Preferably, described selection Adsorption of Cu
2+The appropriate pH value be 5.
Preferably, described magnetic separator is a high gradient magnetic separator.
Preferably, in the 3rd step, the desorption that utilizes the pairing best desorbing agent of concrete metal ion to carry out metal ion is handled.
Preferably, precious metal ion Au
3+Pairing best desorbing agent is a thiocarbamide.
Preferably, precious metal ion Cu
2+Pairing best desorbing agent is ethylene dinitrilotetra-acetic acid EDTA.
By above technical scheme provided by the invention as seen, the present invention utilizes the adsorptivity and the magnetotaxis of magnetotactic bacteria, in conjunction with magnetic separation technique, the thalline that has adsorbed metal ion is carried out solid-liquid separation, the isolated magnetotactic bacteria that is adsorbed with precious metal ion being carried out the desorption of metal ion handles, if adopt electrolytic process to be further purified recovery, obtain the noble metal in the waste water the most at last.By implementing technical scheme of the present invention, can guarantee to effectively utilize the precious metal ion that reclaims in the waste water solution under the prerequisite of efficient, environmental protection.
In addition, the present invention goes back the Au of emphasis to two metal ion species
3+, Cu
2+Adsorption law and recovery scheme are introduced, and by specific embodiments of the invention as can be known, the present invention can reclaim the two kinds of noble metals of gold, copper in the waste water efficiently.
Description of drawings
Fig. 1 is the absorption of precious metal ion in the recovery waste water provided by the invention and the magnetic separation coupling method synoptic diagram to the competitive adsorption sepn process of binary metal ionic system;
Fig. 2 is that the magnetotactic thalline is to Au in monobasic, binary and monobasic, the ternary system
3+, Cu
2+And Ni
2+Adsorption rate with the synoptic diagram of the changing conditions of initial concentration solution; (a) Au
3+-Cu
2+Single component and bicomponent system, (b) Au
3+-Cu
2+-Ni
2+Single component and three compositions system;
Fig. 3 is for serving as the utilization absorption of the present invention of example and the process flow diagram of magnetic separation coupling method with gold, two kinds of noble metal examples of copper.
Embodiment
In order to make those skilled in the art person understand the present invention program better, be described in further detail below in conjunction with the absorption and the magnetic separation coupling method of drawings and embodiments to precious metal ion in the recovery waste water provided by the invention.
A kind of absorption and magnetic separation coupling method that reclaims precious metal ion in the waste water provided by the invention, at first utilize magnetotactic bacteria absorption precious metal ion, utilize high-gradient magnetic field that the magnetotactic bacteria behind the adsorbing metal ions is separated from solution effectively then, comprise the steps:
The first step, in adsorber, select precious metal ion in the adsorbent solution with magnetotactic bacteria.
In the present invention, the first step is specially: contain the pH value of the solution of precious metal ion by adjusting, select precious metal ion in the adsorbent solution with magnetotactic bacteria in adsorber.
At present, the biological particles volume of free state is little, and physical strength is low, is difficult to separate from solution behind the absorption metal, makes biological adsorption technology still rest on laboratory stage mostly.But, magnetotactic bacteria can remedy the above-mentioned shortcoming of general biosorption process, because magnetotactic bacteria not only has good adsorptivity to metal ion, and have unique magnetotaxis, thereby magnetotactic bacteria can separate the organism behind the adsorbing metal ions by high-gradient magnetic field effectively from solution.
This step of selecting to adsorb the precious metal ion in the waste water solution with magnetotactic bacteria is specially:
Adjusting contains the pH value of the solution of precious metal ion, adds a certain amount of magnetotactic bacteria bacterium liquid then, and carries out the adsorption process of magnetotactic bacteria to precious metal ion in the freezing shaking table of constant temperature.
When comprising multiple precious metal ion in the solution, contain the pH value of the solution of precious metal ion by adjusting, realize selecting the absorption precious metal ion by magnetotactic bacteria.
Need to prove that pH has very big influence to the activity of the precious metal ion in the solution.
Specifically experimentally, can be at first the solution of the metal ion for preparing be poured in the adsorber, regulated pH value and temperature, carry out adsorption experiment.Through after the absorption of certain hour, the solution of the 10ml that can take a sample filters through millipore filtration (aperture 0.22 μ m), and measures the content of residual metal ions in the solution with atomic absorption spectrophotometer.
Second goes on foot, utilizes the magnetotactic bacteria magnetic separator is isolated adsorbing metal ions from the mixed solution that the first step obtains after.
In second step, be preferably and adopt high gradient magnetic separator to come magnetotactic bacteria to adsorbing metal ions in the metal ion waste liquid to carry out thalline to capture and peel off.For high gradient magnetic separator, it has the separation efficiency height, and velocity of separation is fast, the advantage that floor space is little.
Absorption separates the coupled detailed process and comprises with magnetic: magnetotactic bacteria before entering magnetic separator with the waste liquid thorough mixing of metal ion, magnetotactic bacteria adsorbs precious metal ion in this process, the waste liquid that carries disease germs then enters magnetic separator, the magnetotactic bacteria that will adsorb metal ion by magnetic field is separated from waste liquid, both reclaim metal ion, purified waste liquid again.This coupling technique to the competitive adsorption sepn process of binary metal ionic system as shown in Figure 1.
As shown in Figure 1, the waste liquid of metal ion and magnetotactic bacteria MTB (Magnetotactic Bacterium) join through pipeline 1 and 4 respectively and carry out the absorption first time in the adsorber 2, discharging is sent into first magnetic separator 8 by peristaltic pump 6 through pipeline 7 through pipeline 5, after separating for the first time through magnetic separator 8, liquid is entered in the adsorber 10 by pipeline 9, in adsorber 10, mix with the magnetotactic bacteria MTB that adds by charging opening 11, carry out the absorption second time, the effluent liquid 12 of adsorber 10 is sent into second magnetic separator 15 by peristaltic pump 13 through pipeline 14, carry out the second time and separate, the solution behind the isolation of purified flows out from pipeline 16.This two discharges the magnetotactic bacteria of metal ion from the pipeline 18 of the pipeline 17 of first magnetic separator 8 and second magnetic separator 15 respectively after magnetic separates.Shown in Figure 13 is agitator.
The 3rd step, the desorption that the isolated magnetotactic bacteria that is adsorbed with precious metal ion of second step is carried out metal ion are handled, if adopt electrolytic process to be further purified recovery, obtain the noble metal in the waste water the most at last.
Because coming that by magnetic separator the magnetotactic bacteria that has adsorbed metal ion in the metal ion waste liquid is carried out thalline captures and peels off, after thalline is peeled off, in this step, the desorption that utilizes the pairing best desorbing agent of concrete metal ion to carry out metal ion is handled.
In the present invention, precious metal ion Au cited below
3+Pairing best desorbing agent is a thiocarbamide, precious metal ion Cu
2+Pairing best desorbing agent is ethylene dinitrilotetra-acetic acid (EDTA).
For the precious metal ion Au that will mention below the present invention
3+And Cu
2+, the concrete operations in described the 3rd step are:
For precious metal ion Au
3+, treat the isolating precious metal ion Au that is adsorbed with of magnetic separator
3+Magnetotactic bacteria reach capture saturated after, separate thalline, utilize thiocarbamide that it is carried out desorption and handle, adopt electrolytic process to be further purified afterwards and reclaim gold.
For precious metal ion Cu
2+, treat the isolating precious metal ion Cu that is adsorbed with of magnetic separator
2+Magnetotactic bacteria reach capture saturated after, peel off the magnetotactic bacteria thalline, and adopt ethylene dinitrilotetra-acetic acid (EDTA) that it is carried out desorption, adopt electrolytic process to be further purified recovery copper again.
Provide the absorption of adopting precious metal ion in the recovery waste water of the present invention and the absorption that magnetic separation coupling method carries out the absorption of single precious metal ion, multiple metal ion below and with the specific embodiment of golden, two kinds of valuable gold ions of copper absorption removal process that is example:
Embodiment one:
Magnetotactic bacteria MTB-3 (Magnetotactic Bacterium) detects embodiment to the adsorption effect of single precious metal ion.
At first, the solution that the 50mL for preparing is contained the single precious metal ion of 80mg/L is poured in the adsorber, the pH value of regulator solution, then, add MTB-3, be mixed with the wet bacteria concentration of 10g/L, and seal charging opening with tampon, in the freezing shaking table of constant temperature, 25 ℃ of following constant temperature 1 hour.Subsequently, sampling 10ml filters through millipore filtration (aperture 0.22 μ m), measures the content of precious metal ion with HITACHI (Hitachi) 180-80 type atomic absorption spectrophotometer, and the concrete adsorption effect of being measured is as shown in table 1:
The adsorption effect that table 1 MTB-3 thalline has respectively multiple metal ion
| Metal ion | Au 3+ | Pd 2+ | Ag + | Pt 4+ | Cu 2+ | Ni 2+ |
| |
2 | 5 | 2 | 2 | 5 | 5 |
| Adsorption rate (%) | 99.5 | 99.2 | 99.0 | 85.9 | 98.4 | 92.1 |
The method of calculation of adsorption rate Y are as follows
In the formula: C
In, C
OutGOLD FROM PLATING SOLUTION belongs to ionic concentration before and after the representative absorption respectively.
As can be seen from the table, the MTB-3 thalline is to precious metal Au
3+, Ag
+, Pd
2+, Pt
4+And heavy metal Cu
2+, Ni
2+Adsorption effect all relatively good, illustrate that the MTB-3 bacterium has certain absorption universality to noble metal, especially to precious metal Au
3+, Ag
+, pd
2+Adsorption rate all reach 99%.
Embodiment 2:
The MTB-3 bacterium is to the detection embodiment of the competitive adsorption characteristic of multiple metal ion coexistence system.
According to the experimental technique of being introduced in the foregoing description one, carried out containing Au
3+, Cu
2+And Ni
2+Two components and the adsorption experiment of three compositions system.On the specific implementation, preparation 50mL contains single precious metal ion of 80mg/L or the many metal ion solution of each 80mg/L in adsorber at every turn.
For single Au solion, regulating its pH value is 2; For the solution that comprises Cu, Ni two components, regulate its pH value to 5; And, regulate its pH value to 2 for the solution that comprises Au, Cu, Ni three components.Add magnetotactic bacteria MTB-3 then, be mixed with the wet bacteria concentration of 10g/L, seal charging opening, in the freezing shaking table of constant temperature, 25 ℃ of following constant temperature 1 hour with tampon.Referring to Fig. 2, Fig. 2 is that the magnetotactic thalline is to Au in monobasic, binary and monobasic, the ternary system
3+, Cu
2+And Ni
2+Adsorption rate with the synoptic diagram of the changing conditions of initial concentration solution.
As can be seen from Figure 2, thalline is to the Au in the unit system
3+(pH=2.0), Cu
2+(pH=5.0) and Ni
2+(pH=5.0) good adsorption effect is all arranged; And in binary and ternary system, the pH value of regulating whole absorption system is 2.0, and this moment, the influence of pH added the competitive adsorption between each metal ion in the multicomponent system, thereby had realized that thalline is to Au
3+Preferential selection absorption, and suppress Cu
2+And Ni
2+Absorption.
Embodiment 3:
Specific embodiment with gold, two kinds of valuable gold ions of copper absorption removal process that is example.
Containing Au
3+-Cu
2+In two component solutions, the pH value of regulator solution is 2, and magnetotactic bacteria MTB-3 is to Au
3+The adsorptive capacity maximum, and to Cu
2+Adsorptive capacity be suppressed; If regulating the pH value is 5, then Cu
2+The adsorptive capacity maximum.Therefore, proposed to comprise that regulating the pH value selects adsorbing metal ions Au
3+And recovery is golden, adsorbing metal ions Cu
2+And the absorption and the magnetic separation coupling technology in recovery two stages of copper.
Concrete technical process is referring to Fig. 3, and Fig. 3 is the absorption magnetic separation coupling method process flow diagram that is example with gold, two kinds of noble metal examples of copper, among Fig. 3, and C
0Refer to that GOLD FROM PLATING SOLUTION belongs to the ionic starting point concentration; C
1, C
2, C
3And C
4Represent that respectively one-level absorption, the separation of one-level magnetic, secondary absorption, secondary magnetic separate the ionic concn in the solution of back.With gold, two kinds of noble metal examples of copper is that the absorption of the present invention of example and the technical process of magnetic separation coupling method are divided into two stages:
Fs is that magnetotactic bacteria is from Au
3+-Cu
2+PH value by regulator solution in the binary system realizes Au
3+Selection absorption, carry out one-level magnetic afterwards and separate.Magnetic separator constantly captures thalline, wait to capture saturated after, separate thalline, utilize thiocarbamide that it is carried out desorption and handle, adopt electrolytic process to be further purified afterwards and reclaim gold.
Subordinate phase is at first suitably replenished a part of magnetotactic bacteria, to remaining Cu in the solution in the solution behind flash trapping stage
2+Adsorb, carry out secondary magnetic afterwards and separate.Equally, treat magnetic separator reach capture saturated after, peel off thalline, adopt ethylene dinitrilotetra-acetic acid (EDTA) that it is carried out desorption.
Utilize absorption to separate coupling technique, to containing Au with magnetic
3+, Cu
2+Solution see table the condition shown in 2 and handle:
The isolating operational condition of table 2 absorption, desorption and magnetic
M represents bacterial concentration in the table, H
0The expression magneticstrength, u
0It is the flow through flow velocity of magnetic separator of treatment solution.V
dThe volume of expression desorption liquid.
Ginseng is shown in Table 3, and table 3 has shown absorption at different levels, separation and desorption treatment effect.
Table 3 absorption, separation and desorption treatment effect
Technical scheme by the invention described above and specific embodiment are as can be known, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water provided by the invention, utilize magnetotactic bacteria absorption precious metal ion earlier, utilize high-gradient magnetic field that the organism behind the adsorbing metal ions is separated from solution effectively then, can guarantee to effectively utilize the precious metal ion that reclaims in the waste water solution under the prerequisite of efficient, environmental protection.
The above only is a preferred implementation of the present invention; should be pointed out that for those skilled in the art, under the prerequisite that does not break away from the principle of the invention; can also make some improvements and modifications, these improvements and modifications also should be considered as protection scope of the present invention.
Claims (8)
1, a kind of absorption and magnetic separation coupling method that reclaims precious metal ion in the waste water is characterized in that, may further comprise the steps:
The first step, in adsorber, select precious metal ion in the adsorbent solution with magnetotactic bacteria;
Second goes on foot, utilizes the magnetotactic bacteria magnetic separator is isolated adsorbing metal ions from the mixed solution that the first step obtains after;
The 3rd step, the desorption that the isolated magnetotactic bacteria that is adsorbed with precious metal ion of second step is carried out metal ion are handled, if adopt electrolytic process to be further purified recovery, obtain the noble metal in the waste water the most at last.
2, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 1, it is characterized in that, the described the first step is specially: contain the pH value of the solution of precious metal ion by adjusting, select precious metal ion in the adsorbent solution with magnetotactic bacteria in adsorber.
3, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 2 is characterized in that, select absorption Au
2+The appropriate pH value be 2.
4, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 2 is characterized in that, select Adsorption of Cu
2+The appropriate pH value be 5.
5, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 1 is characterized in that described magnetic separator is a high gradient magnetic separator.
6, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 1 is characterized in that, in the 3rd step, the desorption that utilizes the pairing best desorbing agent of concrete metal ion to carry out metal ion is handled.
7, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 6 is characterized in that precious metal ion Au
3+Pairing best desorbing agent is a thiocarbamide.
8, the absorption and the magnetic separation coupling method of precious metal ion in the recovery waste water as claimed in claim 6 is characterized in that precious metal ion Cu
2+Pairing best desorbing agent is ethylene dinitrilotetra-acetic acid EDTA.
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101921030A (en) * | 2010-08-05 | 2010-12-22 | 南京大学 | Device for processing heavy metal in garbage percolate |
| CN102070288A (en) * | 2010-12-06 | 2011-05-25 | 河海大学 | Device and method used for restoring sludge polluted by heavy metals |
| CN102701511A (en) * | 2011-03-28 | 2012-10-03 | 上海鑫洲生物科技有限公司 | Method and apparatus for wastewater treatment and heavy metal recycling by non-stationary type bio-adsorbent |
| CN103613161A (en) * | 2013-11-27 | 2014-03-05 | 清华大学 | Device for treating waste water containing arsenic and chromium |
| CN103641214A (en) * | 2013-12-10 | 2014-03-19 | 北京科技大学 | Method for treating heavy metal wastewater by superconductive HGMS (high gradient magnetic separation)-FeOOH coupled technique |
| CN103641215A (en) * | 2013-12-10 | 2014-03-19 | 北京科技大学 | Method for treating heavy metal wastewater by superconductive HGMS (high gradient magnetic separation)-loaded Fe adsorption coupled technique |
| CN104937119A (en) * | 2013-01-21 | 2015-09-23 | 三菱丽阳株式会社 | Method for metal concentration, method for metal recovery, device for metal concentration, and device for metal recovery |
| CN107324616B (en) * | 2017-08-31 | 2018-07-24 | 衡水睿韬环保技术有限公司 | A kind for the treatment of process of heavy metal containing sewage |
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2008
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101921030A (en) * | 2010-08-05 | 2010-12-22 | 南京大学 | Device for processing heavy metal in garbage percolate |
| CN101921030B (en) * | 2010-08-05 | 2012-07-18 | 南京大学 | Device for processing heavy metal in garbage percolate |
| CN102070288A (en) * | 2010-12-06 | 2011-05-25 | 河海大学 | Device and method used for restoring sludge polluted by heavy metals |
| CN102701511A (en) * | 2011-03-28 | 2012-10-03 | 上海鑫洲生物科技有限公司 | Method and apparatus for wastewater treatment and heavy metal recycling by non-stationary type bio-adsorbent |
| CN104937119A (en) * | 2013-01-21 | 2015-09-23 | 三菱丽阳株式会社 | Method for metal concentration, method for metal recovery, device for metal concentration, and device for metal recovery |
| CN103613161A (en) * | 2013-11-27 | 2014-03-05 | 清华大学 | Device for treating waste water containing arsenic and chromium |
| CN103641214A (en) * | 2013-12-10 | 2014-03-19 | 北京科技大学 | Method for treating heavy metal wastewater by superconductive HGMS (high gradient magnetic separation)-FeOOH coupled technique |
| CN103641215A (en) * | 2013-12-10 | 2014-03-19 | 北京科技大学 | Method for treating heavy metal wastewater by superconductive HGMS (high gradient magnetic separation)-loaded Fe adsorption coupled technique |
| CN103641214B (en) * | 2013-12-10 | 2015-07-29 | 北京科技大学 | The method of superconduction HGMS-FeOOH coupling technique process heavy metal wastewater thereby |
| CN103641215B (en) * | 2013-12-10 | 2015-09-23 | 北京科技大学 | The method of the adsorbing coupled art breading heavy metal wastewater thereby of superconduction HGMS-load Fe |
| CN107324616B (en) * | 2017-08-31 | 2018-07-24 | 衡水睿韬环保技术有限公司 | A kind for the treatment of process of heavy metal containing sewage |
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