CN203754481U - Device for degrading polychlorinated biphenyls in water environment - Google Patents

Device for degrading polychlorinated biphenyls in water environment Download PDF

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CN203754481U
CN203754481U CN201420011047.3U CN201420011047U CN203754481U CN 203754481 U CN203754481 U CN 203754481U CN 201420011047 U CN201420011047 U CN 201420011047U CN 203754481 U CN203754481 U CN 203754481U
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reactor
reaction
dividing plate
water distribution
distribution dividing
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赵林
吕倩倩
丁舒
毛国柱
齐云
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Tianjin University
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Tianjin University
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Abstract

The utility model discloses a device for degrading polychlorinated biphenyls in a water environment. A liquid storage tank is connected with a peristaltic pump pipeline; a peristaltic pump is connected with a bottom pipeline of a reactor; a reaction packing column is arranged in the reactor; a first water distribution division plate and a second water distribution division plate are arranged on the upper and lower end surfaces of the reaction packing column; a heat preservation unit is arranged outside the reactor; the top end of the reactor is respectively connected with an outflow pipe and a backflow pipe by virtue of pipelines, and is connected with the liquid storage tank by virtue of the backflow pipe; a first sampling opening, a second sampling opening and a third sampling opening are formed in the vertical direction of the reactor from bottom to top in sequence. By adopting the structure of the device disclosed by the utility model, a solution containing polychlorinated biphenyls can be circularly subjected to treatment of the reaction packing column, so that the device has high degradation rate on a persistent pollutant PCB (polychlorinated biphenyl) in the water environment, and is relatively low in treatment cost without causing secondary pollution.

Description

The device of polychlorobiphenyl in a kind of degradation water environment
Technical field
The utility model belongs to the recovery technique field of water environment pollution, more particularly, relates to the harmless treatment of polychlorinated biphenyl material in water surrounding, is specially one and utilizes the device of polychlorobiphenyl in Ni-Fe duplex metal nano granule degradation water environment.
Background technology
Polychlorobiphenyl (PolychlorinatedBiphenyls is called for short PCBs) is a kind of typical persistence organic pollutant in environment.Because it has higher unreactiveness, thermostability, flame retardant resistance, thermal conductivity and insulativity, be once widely used in the fields such as power industry, Plastics Processing Industry, chemical industry and printing.According to the World Health Organization (WHO) statistics, since eighties of last century starts production the twenties, to the end of the eighties, the whole world has produced approximately 2 × 10 altogether 7t Industrial PC Bs, wherein approximately 31% is discharged in environment.Because PCBs has biological accumulation and " three cause " effect, long-distance migration in the world, and in its migration, conversion process, can be bioaccumulation amplification, its concentration level may improve even hundreds of times of decades of times, and ecotope and HUMAN HEALTH are produced to threat greatly.United Nations Environment Programme (UNEP) is classified as one of preferential 12 kinds of persistence toxic organic pollutants controlling in the whole world, and most industry country is after 20 century 70s, stop producing polychlorobiphenyl, but due to its stable in properties, be difficult for degrading in environment, polychlorobiphenyl also will continue a very long time to the pollution of environment.
The ubiquity existing in water body in view of PCBs, Chinese scholars has been carried out a series of research for the degraded of PCBs in recent ten years, research shows, the committed step of PCBs degraded is dechlorination reaction, and the method for employing mainly contains hydride process, chlorinolysis method, reversion method and metal deoxidization etc.Wherein, utilizing metal deoxidization to process polychlorobiphenyl is a current most active investigative technique, has very large potential, is even considered to have most abroad one of method of application prospect.Zero-valent metal is owing to having very strong reductibility, and cheap and easy to get, therefore can be used as reductive agent, makes polychlorobiphenyl slough chlorine atom, thereby reduces the toxicity of polychlorobiphenyl.Conventional zero-valent metal has iron, aluminium, magnesium, zinc and tin etc., in numerous zero-valent metals, utilize Zero-valent Iron and compound reduction thereof to remove the most study of organic halide and polychlorobiphenyl, and iron is safe from harm for environment, so become more conventional polychlorobiphenyl catalysis dechlorination method.
Metal deoxidization has good application prospect aspect polychlorobiphenyl in removal water surrounding.Grittini research shows, under normal temperature and pressure conditions, Zero-valent Iron is generally difficult to react with polychlorobiphenyl, if but use Pd/Fe combination just can make the dechlorination of polychlorobiphenyl fast restore.Wherein Pd has played the effect of catalysis dechlorination.Expensive due to Pd, can consider to replace Pd as catalyzer with Ni, also can reach higher Degradation Level.Ni/Fe duplex metal nano granule cost is lower, preparation technology is simple and easy to control, and reaction conditions gentleness is removed polychlorobiphenyl speed high, reaction times has also shortened much than fe, and therefore Ni/Fe duplex metal nano granule has larger application prospect in the time processing in water surrounding PCBs.In order to increase the applicability of pollution substance in Ni/Fe duplex metal nano granule degradation water environment, design a kind of packed column circulation type reactor, Ni/Fe duplex metal nano granule is fixed in the middle of filler, avoid duplex metal nano granule to be entrained in water body, cause secondary pollution, this device has larger application prospect.
Utility model content
The purpose of this utility model is to overcome the deficiencies in the prior art, for the water body that contains polychlorobiphenyl, the method that provides one to utilize Ni-Fe duplex metal nano granule degradation of polychlorinated biphenyl, after the immobilization of Ni/Fe duplex metal nano granule, provides a kind of device that more has using value.
Technical purpose of the present utility model is achieved by following technical proposals:
One is utilized the device of polychlorobiphenyl in Ni-Fe duplex metal nano granule degradation water environment, comprises liquid storage tank, peristaltic pump, and the first water distribution dividing plate, the second water distribution dividing plate, reaction-filling post, heat-insulation unit, outflow tube, return line and reactor, wherein:
Described liquid storage tank is connected with peristaltic pump pipeline, and described peristaltic pump is connected with the bottom pipeline of reactor;
Reaction-filling post is set in described reactor, and at the lower surface place of described reaction-filling post, the first water distribution dividing plate is set, the second water distribution dividing plate is set in the upper end surface of described reaction-filling post;
In the outer setting heat-insulation unit of described reactor, it utilizes temperature sensor and heat hot galvanic couple to heat and temperature control being provided with the reactor of reaction-filling post, so that the temperature kept stable of reaction-filling post;
The top of described reactor is connected with return line with outflow tube respectively by pipeline, and the top of described reactor is connected with liquid storage tank by return line.
In above-mentioned reaction unit, bottom-up the first thief hole, the second thief hole and the 3rd thief hole of setting gradually in the vertical direction of reactor, described the first thief hole is arranged on the below of the first water distribution dividing plate, centre and the 3rd thief hole that the second thief hole is arranged on reaction-filling post is arranged on the top of the second water distribution dividing plate, to the water of the reactor of flowing through is sampled to detection.
In above-mentioned reaction unit, described reaction-filling post accounts for 3/5-2/3 of whole reactor volume, adopting Ni-Fe duplex metal nano granule and quartz sand to mix forms, the mixed volume of wherein said Ni-Fe duplex metal nano granule and quartz sand is than being 1:(8-12), preferably adopt mechanical stirring mode to mix; Described quartz sand is 60-80 orders, and the particle of described Ni-Fe duplex metal nano granule is 40-70nm, and specific surface area is 25-35m 2/ g, is prepared according to following step:
Step 1, is dissolved in the PVP of 5 mass parts in deionized water, obtains mass body volume concentrations and be 10% PVP solution;
Step 2, takes NiCl 26H 2o is dissolved in deionized water, obtains NiCl 2solution;
Step 3, gets the NiCl that PVP solution that step 1 obtains and step 2 obtain 2solution, then add deionized water and ethanol, obtains mixing solutions, and passes into deoxygenation after rare gas element, the PVP solution that wherein step 1 obtains, the NiCl that step 2 obtains 2the volume ratio of solution, deionized water and ethanol is (7-8): 1:(20-22): 20, preferably 7.5:1:21.5:20, described rare gas element is selected nitrogen, argon gas or helium, and the deoxygenation time is 20-30min;
Step 4, takes FeSO 47H 2o adds in the mixing solutions that step 3 obtains, and fully dissolves, and is chosen in rotating speed and is under the mechanical stirring condition of 1500-2000r/min to mix 15-20min, makes FeSO 47H 2o powder fully dissolves;
Step 5 drips NaBH in the solution obtaining in step 4 4solution completes dropping in 15-20min, drips after finishing under the mechanical stirring condition that is 1500-2000r/min at rotating speed and stirs 20-30min, described NaBH 4solution is the NaBH of 0.12-0.13g 4powder is dissolved in percent by volume 40% aqueous ethanolic solution of 10ml, after stirring, obtains;
Step 6, after stirring finishes, after collecting by magnetic method, washing is dried, and can obtain Ni-Fe duplex metal nano granule;
Wherein Fe 2+and BH 4-molar ratio 1:2, for reduction reaction is fully carried out, preferably excessive NaBH 4solution; The consumption of described nickel is 2%-5% of ferrous iron (being ferro element) quality; In technique scheme, a step is achieved as follows whole reaction process:
Fe 2++6H 2O+2BH 4 -→Fe↓+2Be(OH) 3+7H 2↑
Ni 2++6H 2O+2BH 4 -→Ni↓+2Be(OH) 3+7H 2↑
In this course, because the addition of elemental nickel is less and system is fully mixed and reacts under churned mechanically condition continuing, after drop reaction finishes, can form the composite nanometer particle of nickel and iron.Metal Ni plays catalyzer, can accelerate the dechlorination efficiency of Zero-valent Iron, conventionally selects Ni/Fe duplex metal nano granule degradation of polychlorinated biphenyl cheap and easy to get.The liquid phase reduction of selecting has simple to operate, process controllability is strong, cost is the advantage such as lower also, conventionally select sodium borohydride liquid phase reduction to prepare Ni/Fe duplex metal nano granule, but the nano particle of preparing is easily reunited, and affects degradation efficiency, so add stablizer PVP (K30) in liquid phase preparation process, PVP (K30) can prevent the reunion of nanoparticle, also can not exert an influence to the degradation process of bimetal system.
In above-mentioned reaction unit, described reaction unit is airtight on the whole, in order to avoid oxygen enters in reaction unit, Ni-Fe duplex metal nano granule is caused to oxidation, causes speed of reaction greatly to reduce.
In above-mentioned reaction unit, described outflow tube is connected by T-valve with return line.
In above-mentioned reaction unit, on described the first water distribution dividing plate and the second water distribution dividing plate, be uniformly distributed water distributing pore, the aperture of described water distributing pore is 0.01mm-0.3mm; For preventing the seepage of quartz sand and Ni-Fe duplex metal nano granule, in the one side contacting with reaction-filling post of described the first water distribution dividing plate and the second water distribution dividing plate, gauze is set; The material of described the first water distribution dividing plate and the second water distribution dividing plate is synthetic glass, and thickness is 3-5mm.
Utilize the method for polychlorobiphenyl in above-mentioned reaction unit degradation water environment, carry out according to following step:
Step 1, is placed in liquid storage tank by the solution that contains polychlorobiphenyl, and opens peristaltic pump;
Step 2, described in contain polychlorobiphenyl solution entered by reactor bottom, after water-distributing device water distribution uniformity, by reaction-filling post;
Step 3, the state of adjustment T-valve, so that the solution that contains polychlorobiphenyl is back in liquid storage tank via return line;
Step 4, repeats above-mentioned steps so that the solution that contains polychlorobiphenyl circulates in reactor, and analyzes the removal effect of polychlorobiphenyl by thief hole;
Step 5, in the time that the removal effect of polychlorobiphenyl reaches preset requirement, adjusts the state of T-valve, so that solution is flowed out by outflow tube.
In such scheme, by regulating the Flow-rate adjustment solution of the peristaltic pump hydraulic detention time in reaction-filling post, the hydraulic detention time of each circulation is 60min-90min, and the total hrt of whole reaction is 48-72h.
In such scheme, to move under constant temperature by the whole reaction of heat-insulation unit control, temperature is 30-40 DEG C.
In such scheme, described in contain polychlorobiphenyl solution in, the concentration of polychlorobiphenyl is 3mg/L-5mg/L.
In such scheme, in described reaction unit, comprise that reactor, liquid storage tank, reaction-filling post and pipeline thereof are all pre-
First use rare gas element (as nitrogen, helium, argon gas) to carry out deoxygenation.
The utility model utilizes Ni/Fe duplex metal nano granule, and the pollution by polychlorinated biphenyles thing in efficient degradation water surrounding adopts packed column loop reactor, and flow process is simple, and controllability is strong, and cost is also lower.The method of polychlorobiphenyl in a kind of Ni/Fe of the utilization duplex metal nano granule degradation water environment the utility model proposes, Ni/Fe duplex metal nano granule is fixed in quartz sand filler, when polychlorobiphenyl ethanol-aqueous solution passes through filler continuously, bimetal carries out dechlorination to polychlorobiphenyl.
Brief description of the drawings
Fig. 1 is the structural representation that the utility model one is utilized the device of polychlorobiphenyl in Ni-Fe duplex metal nano granule degradation water environment, and wherein 1 is liquid storage tank, and 2 is peristaltic pump, 3-1 is the first water distribution dividing plate, and 3-2 is the second water distribution dividing plate, and 4 is reaction-filling post, 5 is heat-insulation unit (system), 6 is outflow tube, and 7 is return line, and 8 is T-valve, 9-1 is the first thief hole, 9-2 is the second thief hole, and 9-3 is the 3rd thief hole, and 10 is reactor.
Fig. 2 is the structural representation of the water distribution dividing plate that uses in the utility model, and 11 is water distributing pore.
Fig. 3 is the design sketch while utilizing device of the present utility model to degrade PCB77 ethanol-aqueous solution.
Embodiment
Further illustrate the technical solution of the utility model below in conjunction with specific embodiment.
As shown in accompanying drawing 1-2, utilize the device of polychlorobiphenyl in Ni-Fe duplex metal nano granule degradation water environment, comprise liquid storage tank, peristaltic pump, the first water distribution dividing plate, the second water distribution dividing plate, reaction-filling post, heat-insulation unit, outflow tube, return line and reactor, wherein:
Described liquid storage tank is connected with peristaltic pump pipeline, and described peristaltic pump is connected with the bottom pipeline of reactor;
Reaction-filling post is set in described reactor, and at the lower surface place of described reaction-filling post, the first water distribution dividing plate is set, the second water distribution dividing plate is set in the upper end surface of described reaction-filling post;
In the outer setting heat-insulation unit of described reactor, it utilizes temperature sensor and heat hot galvanic couple to heat and temperature control being provided with the reactor of reaction-filling post, so that the temperature kept stable of reaction-filling post;
The top of described reactor is connected with return line with outflow tube respectively by pipeline, and the top of described reactor is connected with liquid storage tank by return line.
In above-mentioned reaction unit, bottom-up the first thief hole, the second thief hole and the 3rd thief hole of setting gradually in the vertical direction of reactor, described the first thief hole is arranged on the below of the first water distribution dividing plate, centre and the 3rd thief hole that the second thief hole is arranged on reaction-filling post is arranged on the top of the second water distribution dividing plate, to the water of the reactor of flowing through is sampled to detection.
In above-mentioned reaction unit, described reaction unit is airtight on the whole, in order to avoid oxygen enters in reaction unit, Ni-Fe duplex metal nano granule is caused to oxidation, causes speed of reaction greatly to reduce.Described outflow tube is connected by T-valve with return line.On described the first water distribution dividing plate and the second water distribution dividing plate, be uniformly distributed water distributing pore, the aperture of described water distributing pore is 0.1mm-0.3mm; For preventing the seepage of quartz sand and Ni-Fe duplex metal nano granule, in the one side contacting with reaction-filling post of described the first water distribution dividing plate and the second water distribution dividing plate, gauze is set; The material of described the first water distribution dividing plate and the second water distribution dividing plate is synthetic glass, and thickness is 3-5mm.
In above-mentioned reaction unit, described reaction-filling post accounts for 3/5-2/3 of whole reactor volume, adopting Ni-Fe duplex metal nano granule and quartz sand to mix forms, the mixed volume of wherein said Ni-Fe duplex metal nano granule and quartz sand is than being 1:(8-12), preferably adopt mechanical stirring mode to mix; Described quartz sand is 60-80 orders, and the particle of described Ni-Fe duplex metal nano granule is 40-70nm, and specific surface area is 25-35m 2/ g, is prepared according to following step:
(1) 5gPVP (K30) is dissolved in deionized water, fully mixes by magnetic agitation, be settled to 50ml, obtain mass body volume concentrations and be 10% PVP solution.
(2) take the NiCl of metered amount 26H 2o powder, is dissolved in deionized water, obtains its standardized solution.
NiCl 26H 2the quality of O powder determines by Ni/Fe, and the usage quantity of nickel is weight of iron 2-5%, and its metered amount is equivalent to dissolve NiCl in every milliliter of standardized solution 26H 2the quality of O powder is in 0.00168-0.0042 scope.NiCl 26H 2o and FeSO 47H 2the relation of O is as following table:
(3) get as described in (1) 7.5mlPVP solution, add 1ml (2) NiCl 2standardized solution, deionized water 21.5ml, ethanol 20ml, proceeds in there-necked flask after mixing, letting nitrogen in and deoxidizing 20-30min.Overall solution volume is 50ml.
(4) take 0.417gFeSO 47H 2o powder adds in above-mentioned solution, under the mechanical stirring condition that is 1500-2000r/min, mixes 15-20min at rotating speed, makes FeSO 47H 2o powder fully dissolves, now FeSO 47H 2the volumetric molar concentration of O is 0.03mol/L.
(5) slowly in there-necked flask, drip NaBH 4solution, according to n (Fe 2+) and n (BH 4 -) ratio 1:2, NaBH 4for 0.003mol, consider a small amount of Ni of reduction 2+needs and operating process loss, carry out configuration NaBH for ensureing to react completely 4when solution, claim slightly excessive NaBH 4powder, the NaBH4 powder that weighs 0.12-0.13g is dissolved in 40% ethanolic soln of 10ml, after stirring, obtains NaBH 4solution completes dropping in 15-20min, drips after finishing under the mechanical stirring condition that is 1500-2000r/min at rotating speed and stirs 20-30min.
(6), after stirring and finishing, collect by magnetic method, deoxidation distilled water wash 3-4 times for the Ni-Fe nano particle that obtains, absolute ethanol washing 1-2 times, can the auxiliary washing of ultrasonic dispersion to remove residual ion and organism in solution.After washing finishes, collect by magnetic method, the Ni/Fe duplex metal nano granule obtaining, through vacuum-drying, weighs, and is about 0.1g left and right.
Obtain the concentration of the PCB77 of each sampling spot by GC-ECD Instrument measuring, the concentration of 0h is designated as initial concentration C 0, the concentration recording is afterwards designated as measurement concentration C, and degradation rate calculates by following formula, as shown in Figure 3.
The solution that contains polychlorobiphenyl is the ethanol-aqueous solution of polychlorobiphenyl, selects PCB77 to implement as target contaminant, the reaction-filling post that Ni/Fe duplex metal nano granule prepared by use aforesaid method and quartz sand mix.
Embodiment 1
The small aperture of water distribution dividing plate is 0.01mm, and in reaction-filling post, the floor height of quartz sand accounts for 3/5 of whole cylinder.Before liquid storage tank adds PCB77 ethanol-aqueous solution, whole device in advance logical nitrogen makes it in anaerobic environment, and in whole reaction process, reaction unit keeps the constant temperature of 30 DEG C by heat-insulation system.Reaction-filling post is put into the uniform mixture of quartz sand and Ni/Fe duplex metal nano granule in advance, and blending ratio is 1:9.In liquid storage tank, adding concentration is PCB77 ethanol-aqueous solution of 5mg/L, and this solution also carried out letting nitrogen in and deoxidizing in advance.Open peristaltic pump, making the residence time of solution in filled column is 60min, changes, when in 48h, solution is by reaction filled column in the 3rd thief hole sampling and measuring PCB77 strength of solution, outflow tube is all in closure state, and solution is back to liquid storage tank by return line.In the time that the reaction times is 48h, closed return line, starts outflow tube, and reaction finishes.In reaction process, observe the change in concentration of PCB77 solution in the 3rd thief hole position, finally recording degradation efficiency is 88%.
Embodiment 2
The small aperture of water distribution dividing plate is 0.1mm, and in reaction-filling post, the floor height of quartz sand accounts for 3/5 of whole cylinder.Before liquid storage tank adds PCB77 ethanol-aqueous solution, whole device in advance logical nitrogen makes it in anaerobic environment, and in whole reaction process, reaction unit keeps the constant temperature of 40 DEG C by heat-insulation system.Reaction-filling post is put into the uniform mixture of quartz sand and Ni/Fe duplex metal nano granule in advance, and blending ratio is 1:12.In liquid storage tank, adding concentration is PCB77 ethanol-aqueous solution of 5mg/L, and this solution also carried out letting nitrogen in and deoxidizing in advance.Open peristaltic pump, making the residence time of solution in filled column is 90min, changes, when in 60h, solution is by reaction filled column in the 3rd thief hole sampling and measuring PCB77 strength of solution, outflow tube is all in closure state, and solution is back to liquid storage tank by return line.In the time that the reaction times is 60h, closed return line, starts outflow tube, and reaction finishes.In reaction process, observe the change in concentration of PCB77 solution in the 3rd thief hole position.Finally recording degradation efficiency is 93%.
Embodiment 3
The small aperture of water distribution dividing plate is 0.3mm, and in reaction-filling post, the floor height of quartz sand accounts for 2/3 of whole cylinder.Before liquid storage tank adds PCB77 ethanol-aqueous solution, whole device in advance logical nitrogen makes it in anaerobic environment, and in whole reaction process, reaction unit keeps the constant temperature of 35 DEG C by heat-insulation system.Reaction-filling post is put into the uniform mixture of quartz sand and Ni/Fe duplex metal nano granule in advance, and blending ratio is 1:8.In liquid storage tank, adding concentration is PCB77 ethanol-aqueous solution of 5mg/L, and this solution also carried out letting nitrogen in and deoxidizing in advance.Open peristaltic pump, making the residence time of solution in filled column is 80min, changes, when in 72h, solution is by reaction filled column in the 3rd thief hole sampling and measuring PCB77 strength of solution, outflow tube is all in closure state, and solution is back to liquid storage tank by return line.In the time that the reaction times is 72h, closed return line, starts outflow tube, and reaction finishes.In reaction process, observe the change in concentration of PCB77 solution in the 3rd thief hole position.Finally recording degradation efficiency is 97.4%.
Above the utility model is done to exemplary description; should be noted that; in the situation that not departing from core of the present utility model, the replacement that is equal to that any simple distortion, amendment or other those skilled in the art can not spend creative work all falls into protection domain of the present utility model.

Claims (5)

1. a device for polychlorobiphenyl in degradation water environment, is characterized in that, described device is airtight on the whole, comprises liquid storage tank, peristaltic pump, and the first water distribution dividing plate, the second water distribution dividing plate, reaction-filling post, heat-insulation unit, outflow tube, return line and reactor, wherein:
Described liquid storage tank is connected with peristaltic pump pipeline, and described peristaltic pump is connected with the bottom pipeline of reactor; Reaction-filling post is set in described reactor, and at the lower surface place of described reaction-filling post, the first water distribution dividing plate is set, the second water distribution dividing plate is set in the upper end surface of described reaction-filling post; In the outer setting heat-insulation unit of described reactor; The top of described reactor is connected with return line with outflow tube respectively by pipeline, and the top of described reactor is connected with liquid storage tank by return line; Bottom-up the first thief hole, the second thief hole and the 3rd thief hole of setting gradually in the vertical direction of reactor, described the first thief hole is arranged on the below of the first water distribution dividing plate, centre that the second thief hole is arranged on reaction-filling post and the 3rd thief hole and is arranged on the top of the second water distribution dividing plate.
2. the device of polychlorobiphenyl in a kind of degradation water environment according to claim 1, is characterized in that, described reaction-filling post accounts for 3/5-2/3 of whole reactor volume.
3. the device of polychlorobiphenyl in a kind of degradation water environment according to claim 1, is characterized in that, described outflow tube is connected by T-valve with return line.
4. the device of polychlorobiphenyl in a kind of degradation water environment according to claim 1, it is characterized in that, on described the first water distribution dividing plate and the second water distribution dividing plate, be uniformly distributed water distributing pore, the aperture of described water distributing pore is 0.01mm-0.3mm, and the thickness of described the first water distribution dividing plate and the second water distribution dividing plate is 3-5mm.
5. the device of polychlorobiphenyl in a kind of degradation water environment according to claim 4, is characterized in that, with in the one side contacting with reaction-filling post on the second water distribution dividing plate, gauze is set at described the first water distribution dividing plate.
CN201420011047.3U 2014-01-02 2014-01-02 Device for degrading polychlorinated biphenyls in water environment Expired - Fee Related CN203754481U (en)

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