CN104192978A - Optoacoustic synergic perfluorooctane sulfonate (PFOS) degradation device and method - Google Patents

Optoacoustic synergic perfluorooctane sulfonate (PFOS) degradation device and method Download PDF

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CN104192978A
CN104192978A CN201410425097.0A CN201410425097A CN104192978A CN 104192978 A CN104192978 A CN 104192978A CN 201410425097 A CN201410425097 A CN 201410425097A CN 104192978 A CN104192978 A CN 104192978A
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reactor
pfos
water
ultrasonic generator
ultraviolet lamp
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CN104192978B (en
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程建华
梁小燕
郑华生
张鹏
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South China University of Technology SCUT
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Abstract

The invention discloses an optoacoustic synergic perfluorooctane sulfonate (PFOS) degradation device and method. The device comprises an ultrasonic generator and a water tank which is arranged on the ultrasonic generator and used for keeping reaction temperature, wherein a reactor for containing wastewater containing potassium perfluorooctane sulfonate is arranged in the water tank; an ultraviolet lamp is arranged above the reactor; and the reactor is made from an inert material. The method comprises the following steps: a) adding the wastewater containing PFOS to be treated into the reactor, adding heteropoly acid as a catalyst, and adding H2O2 to control the pH value at 2-4; and b) turning on the ultraviolet lamp and ultrasonic generator, reacting under the ultrasonic power of 100W for 3-5 hours, and discharging. The device is simple in structure; and the UV-US/H3PW12O40 optoacoustic synergic catalytic oxidation system fully displays the strong decomposition effect of the 358 kHz ultrasonic and the photocatalysis action of the heteropoly acid under the 254nm ultraviolet irradiation, thereby implementing effective degradation and defluorination of the PFOS.

Description

A kind of apparatus and method of optoacoustic Synergistic degradation perfluoro octane sulfonate
Technical field
The invention belongs to environmental engineering water-treatment technology field, is about treatment unit and the method for the perfluorochemicals such as persistence organic pollutant perfluoro octane sulfonate (PFOS) in water body, is specially a kind of based on UV-US/H 3pW 12o 40the apparatus and method of Perfluorooctane sulfonates potassium (PFOS) in system concerted catalysis oxidative degradation water.
Background technology
Perfluorochemical (PFCs) is widely used in industry and the civil areas such as weaving, papermaking, packing, agricultural chemicals, carpet, leather, polishing floor, shampoo and fire foam.The PFCs existing in environment mainly contains perfluori piated carboxylic acids, perfluorinated sulfonic acid class, perfluor amides and perfluor telomeric alcohol etc., and Perfluorocaprylic Acid (PFOA) is current most widely used perfluor organism with perfluoro octane sulfonate (PFOS), PFOS is large compared with PFOA degraded difficulty.Its a large amount of production and use have caused very serious environment accumulation and persistence to pollute in the world's ecosystems.
The C-F key that PFOS has causes its chemical property very stable, not yet finds so far any evidence and relevant report that they are degraded in vivo, does not also find the research of its any natural degradation.Conventional high-level oxidation technology is (as O 3, O 3/ UV, O 3/ H 2o 2and H 2o 2/ Fe 2+) all can not make it effectively degrade.Although at present many investigators have carried out with means such as biological degradation, redox, high temperature incinerations and have removed the research with recovery technology method for different perfluorinated compounds, the drawbacks such as they all exist to some extent, and degradation efficiency is low, speed is slow, energy consumption is high, complicated operation, the rate of recovery are low, secondary pollution.Therefore, at present about the degraded reparation research of PFCs also in the starting stage, only have the research of minority to carry out, as better in subcritical system, photochemical catalysis system degradation effect, but conditional request is higher, energy consumption is large; Photochemical catalytic oxidation system reaction conditions is relatively gentle, but defluorinate process is slow and efficiency is not high; Photoxidation system can cause secondary pollution and the problem of crossing high cost due to the use of a large amount of oxygenants, all the difficult processing for actual waste water.Therefore effective defluorinating and degrading complete of how realizing PFOS is one of urgent problem.
Summary of the invention
The object of the present invention is to provide a kind of based on UV-US/H 3pW 12o 40the apparatus and method of the degraded of Perfluorooctane sulfonates potassium and defluorinate in system catalysed promoted water, this system can realize the efficient degradation of PFOS, improves defluorinate rate, Reaction time shorten.
Object of the present invention is achieved through the following technical solutions:
The device of the degraded of Perfluorooctane sulfonates potassium and defluorinate in the collaborative promotion of a kind of optoacoustic water, this device comprises ultrasonic generator (high frequency) and is placed on ultrasonic generator for keeping the tank of temperature of reaction, in tank, be provided with the reactor containing Perfluorooctane sulfonates potassium waste water for splendid attire, described reactor top is provided with ultraviolet lamp, and this reactor is made by inertia material.
Described ultraviolet lamp is horizontally placed on reactor, and with reactor in the distance of liquid level be 3～5cm.
The power of described ultraviolet lamp is 11W, and the UV-light of transmitting 254nm.
Described ultrasonic generator transmitting frequency is 358kHz, and rated output is 100W.
Described reactor is the cylindrical vessel being made by tetrafluoroethylene, which is provided with stopple coupon, for sampling analysis; Described tank is provided with condensate pipe.
The method of utilizing Perfluorooctane sulfonates potassium in said apparatus degradation water, comprises the steps:
A) the pending waste water containing Perfluorooctane sulfonates potassium is added in reactor, add heteropolyacid (H 3pW 12o 40) as catalyzer, add H 2o 2as oxygenant, control pH value between 2～4;
B) open ultraviolet lamp and ultrasonic generator, it is 100W that ultrasonic power is set, and reacts 3～5 hours, gets final product water outlet.
The mass ratio of described Perfluorooctane sulfonates potassium and heteropolyacid is 1:50～1:150, and the concentration of heteropolyacid is 0.5～1.5g/L.
Described heteropolyacid is phospho-wolframic acid (H 7[P (W 2o 7) 6] XH 2o), analytical pure, is purchased from Tianjin Chemical Co., Ltd.'s all generations.
Described reaction is carried out under the condition of 30～40 ℃ of constant temperature.
The mass ratio of described Perfluorooctane sulfonates potassium and oxygenant is 1:5～1:20.
Wherein, pH is 2 o'clock best results, can be according to definite actual pH such as water quality situation, economy.
The polluted water body that contains PFOS is carried out to pre-treatment, and the water body that turbidity is higher need filter, and in reduction water, suspended substance is to ultraviolet attenuation.Preferably, in pending polluted water body, the concentration range of PFOS is at 5～30mg/L, and the dosage of oxygenant is 50～200mg/L.
Ultraviolet lamp of the present invention needs the cell outside closed reactor while using, and prevents that UV-light from damaging operator around.Add oxygenant H 2o 2system is played a driving role, and this promoter action is improved the regeneration rate of photocatalyst and has been increased oxygen concn in system by oxygenant and realizes.
Compared with prior art, tool has the following advantages in the present invention:
1) apparatus of the present invention is simple in structure, and ultrasonic wave, UV-light and the heteropolyacid catalyst adding form UV-US/H 3pW 12o 40optoacoustic concerted catalysis oxidation system, has given full play to ultrasonic strong Decomposition and the photocatalysis of heteropolyacid under 254nm uv irradiation, has realized effective degraded and the defluorinate of PFOS.
2) reaction conditions is simple: this system ultraviolet lamp power is 11w; System is without out-source gas, and general photochemical catalysis system needs out-source gas to continue air feed, and system of the present invention no requirement (NR) on reaction atmosphere; This system is to temperature-insensitive, and reacting solution pH value can be realized efficient degradation in 2～4 scopes, and reaction conditions is simpler.
3) defluorination effect is good: under same treatment condition, and this UV-US/H 3pW 12o 4the degraded defluorination effect of system is significantly better than independent ultrasonic system and photochemical catalysis system, and defluorinate rate is promoted to more than 75% compared with traditional method is the highest, and defluorinate speed is accelerated.
4) reduce toxicity: ultrasonic wave can shorten the carbon chain lengths of perfluorochemical, reduces its toxicity, reduce residue, its poisonous intermediate product greatly reduces compared with photochemical catalysis system, is conducive to repair the environment that PFOS pollutes.
Accompanying drawing explanation
Fig. 1 is the structural representation of apparatus of the present invention.
Embodiment
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but embodiments of the present invention are not limited to this.
Embodiment 1
Device (the UV/H of the degraded of Perfluorooctane sulfonates potassium and defluorinate in the collaborative promotion of a kind of optoacoustic water 3pW 12o 40system), this device comprises ultrasonic generator 1 and is placed on ultrasonic generator 1 for keeping the tank 3 of temperature of reaction, in tank 3, be provided with the reactor 5 containing Perfluorooctane sulfonates potassium waste water for splendid attire, described reactor 5 tops are provided with low pressure ultraviolet lamp 4, described ultraviolet lamp 4 is horizontally placed on reactor 5, and with reactor 5 in the distance of liquid level be 3cm.Described reactor 5 is the cylindrical vessel that made by tetrafluoroethylene, which is provided with stopple coupon 6.Tank 3 is provided with condensate pipe 2.
The power of described ultraviolet lamp 4 is 11W, and the UV-light of transmitting 254nm.
The ultrapure water that processing contains PFOS, the original pH of water sample is that 6.91, PFOS concentration is 10mg/L, F -concentration is about 0 (not detecting), does not need pre-treatment, can directly degrade.
Utilize the method for PFOS in this device degradation water, only apply in the present embodiment ultraviolet lamp, do not open high frequency ultrasound generating unit, use separately UV/H 3pW 12o 40system degraded PFOS, comprises the steps:
A) by pending adding in reactor 5 containing PFOS waste water, add heteropolyacid, concentration is 1g/L, PFOS/H simultaneously 3pW 12o 40(mass concentration ratio) is 1:100, and wherein a group reaction device adds 200mg/LH 2o 2solution, another group control group does not add H 2o 2solution, two groups of test reacting liquid pH values are adjusted to 2 with 0.1mol/LNaOH and HCl;
B) open UV-light power supply 7, in reaction process, the water in tank 3 relies on condensate pipe 2 to realize continuous flow, in air, under normal pressure, reacts, and without out-source gas, temperature of reaction maintains 30 ℃ by tank 3, and system is reacted 4 hours under the condition of constant temperature;
C) close UV-light power supply 7, close ultrasonic generator 1, reaction finishes, and water outlet adopts chromatography of ions to detect F in water -concentration, determines defluorinate rate.
After testing, do not add H 2o 2time, UV/H 3pW 12o 40the defluorinate rate of system only 9.47%, and add H 2o 2, the defluorinate rate of PFOS reaches 33.33%, illustrates that can promote the photochemical catalysis defluorination effect of PFOS adding of oxygenant.
Embodiment 2
Device (the low frequency US-UV/H of the degraded of Perfluorooctane sulfonates potassium and defluorinate in the collaborative promotion of a kind of optoacoustic water 3pW 12o 40system), this device comprises ultrasonic generator 1 and is placed on ultrasonic generator 1 for keeping the tank 3 of temperature of reaction, in tank 3, be provided with the reactor 5 containing Perfluorooctane sulfonates potassium waste water for splendid attire, described reactor 5 tops are provided with low pressure ultraviolet lamp 4, described ultraviolet lamp 4 is horizontally placed on reactor 5, and with reactor 5 in the distance of liquid level be 3cm.Described reactor 5 is the cylindrical vessel that made by tetrafluoroethylene, which is provided with stopple coupon 6.Tank 3 is provided with condensate pipe 2.
The power of described ultraviolet lamp 4 is 11W, and the UV-light of transmitting 254nm.Described ultrasonic generator 1 is low frequency ultrasound projector, and transmitting frequency is 40kHz, and rated output is 120W.
The ultrapure water that processing contains PFOS, the original pH of water sample is that 6.96, PFOS concentration is 10mg/L, F -concentration is about 0 (not detecting), does not need pre-treatment, can directly degrade.
Utilize the method for PFOS in this device degradation water, adopt independent low frequency ultrasound and low frequency US-UV/H 3pW 12o 40system contrast degraded PFOS, comprises the steps:
A) by pending adding in reactor 5 containing PFOS waste water, add heteropolyacid, concentration is 1g/L, PFOS/H simultaneously 3pW 12o 40(mass concentration ratio) is 1:100, adds 200mg/L H 2o 2solution, pH value is adjusted to 2 with 0.1mol/L NaOH and HCl;
B) open the power supply of ultrasonic wave 1, setting reaction power is 100W, open UV-light power supply 7 simultaneously, and ultraviolet lamp is not opened in control group test, in reaction process, the water in tank 3 relies on condensate pipe 2 to realize continuous flow, in air, under normal pressure, react, without out-source gas, temperature of reaction maintains 30 ℃ by tank 3, and system is reacted 4 hours under the condition of constant temperature;
C) close UV-light power supply 7, close ultrasonic generator 1, reaction finishes, and water outlet adopts chromatography of ions to detect F in water -concentration, determines defluorinate rate.
After testing, directly the degrade defluorinate rate of PFOS of high-frequency ultrasonic is 10.1%, low frequency US-UV/H 3pW 12o 40the defluorinate rate of system reaches 20.4%, but UV/H 3pW 12o 40the defluorinate rate of system has reached 33.33% (seeing embodiment 1), and the introducing that low frequency ultrasound is described is for the PFOS restraining effect of having degraded.
Embodiment 3
Device (the high frequency US-UV/H of the degraded of Perfluorooctane sulfonates potassium and defluorinate in the collaborative promotion of a kind of optoacoustic water 3pW 12o 40system), this device comprises ultrasonic generator 1 and is placed on ultrasonic generator 1 for keeping the tank 3 of temperature of reaction, in tank 3, be provided with the reactor 5 containing Perfluorooctane sulfonates potassium waste water for splendid attire, described reactor 5 tops are provided with low pressure ultraviolet lamp 4, described ultraviolet lamp 4 is horizontally placed on reactor 5, and with reactor 5 in the distance of liquid level be 3cm.Described reactor 5 is the cylindrical vessel that made by tetrafluoroethylene, which is provided with stopple coupon 6.Tank 3 is provided with condensate pipe 2.
The power of described ultraviolet lamp 4 is 11W, and the UV-light of transmitting 254nm.Described ultrasonic generator 1 is high frequency ultrasound producer, and transmitting frequency is 358kHz, and rated output is 100W.
The ultrapure water that processing contains PFOS, the original pH of water sample is that 6.86, PFOS concentration is 10mg/L, F -concentration is about 0 (not detecting), does not need pre-treatment, can directly degrade.
Utilize the method for PFOS in this device degradation water, adopt independent high frequency ultrasound and high frequency US-UV/H 3pW 12o 40system contrast degraded PFOS, comprises the steps:
A) by pending adding in reactor 5 containing PFOS waste water, add heteropolyacid, concentration is 1g/L, PFOS/H simultaneously 3pW 12o 40(mass concentration ratio) is 1:100, adds 200mg/L H 2o 2solution, pH value is adjusted to 2 with 0.1mol/L NaOH and HCl;
B) open the power supply of ultrasonic wave 1, setting reaction power is 100W, open UV-light power supply 7 (high frequency ultrasound system is not opened ultraviolet source separately) simultaneously, in reaction process, water in tank 3 relies on condensate pipe 2 to realize continuous flow, reacts, without out-source gas in air under normal pressure, temperature of reaction maintains 30 ℃ by tank 3, and system is reacted 4 hours under the condition of constant temperature;
C) close UV-light power supply 7, close ultrasonic generator 1, reaction finishes, and water outlet adopts chromatography of ions to detect F in water -concentration, determines defluorinate rate.
After testing, high frequency US-UV/H 3pW 12o 40in system, the defluorinate rate of PFOS reaches 82.5%, and independent ultrasonic system defluorinate rate is 58.5%, UV/H 3pW 12o 40the defluorinate rate of system is 33.3% (seeing embodiment 1), illustrates that the introducing of high frequency ultrasound is conducive to the degraded of PFOS, UV-US/H of the present invention 3pW 12o 4optoacoustic collaboration system has good degradation effect for PFOS, can realize simple condition and be issued to higher defluorinate rate.
Embodiment 4
Device (the high frequency US-UV/H of the degraded of Perfluorooctane sulfonates potassium and defluorinate in the collaborative promotion of a kind of optoacoustic water 3pW 12o 40system), this device comprises ultrasonic generator 1 and is placed on ultrasonic generator 1 for keeping the tank 3 of temperature of reaction, in tank 3, be provided with the reactor 5 containing Perfluorooctane sulfonates potassium waste water for splendid attire, described reactor 5 tops are provided with low pressure ultraviolet lamp 4, described ultraviolet lamp 4 is horizontally placed on reactor 5, and with reactor 5 in the distance of liquid level be 3cm.Described reactor 5 is the cylindrical vessel that made by tetrafluoroethylene, which is provided with stopple coupon 6.Tank 3 is provided with condensate pipe 2.
The power of described ultraviolet lamp 4 is 11W, and the UV-light of transmitting 254nm.Described ultrasonic generator 1 is high frequency ultrasound producer, and transmitting frequency is 358kHz, and rated output is 100W.
The ultrapure water that processing contains PFOS, the original pH of water sample is that 6.90, PFOS concentration is 10mg/L, F -concentration is about 0 (not detecting), does not need pre-treatment, can directly degrade.
Utilize the method for PFOS in this device degradation water, attempt contrast degraded PFOS at differential responses temperature, comprise the steps:
A) by pending adding in reactor 5 containing PFOS waste water, add heteropolyacid, concentration is 1g/L, PFOS/H simultaneously 3pW 12o 40(mass concentration ratio) is 1:100, adds 200mg/L H 2o 2solution, pH value is adjusted to 2 with 0.1mol/L NaOH and HCl;
B) open the power supply of ultrasonic wave 1, setting reaction power is 100W, open UV-light power supply 7 simultaneously, in reaction process, the water in tank 3 relies on condensate pipe 2 to realize continuous flow, in air, under normal pressure, reacts, without out-source gas, temperature of reaction maintains 35 ℃ by tank 3, and another group design temperature is 40 ℃, and system is reacted 4 hours under the condition of constant temperature;
C) close UV-light power supply 7, close ultrasonic generator 1, reaction finishes, and water outlet adopts chromatography of ions to detect F in water -concentration, determines defluorinate rate.
After testing, when temperature of reaction is 35 ℃, high frequency US-UV/H 3pW 12o 40in system, the defluorinate rate of PFOS reaches 84.1%, and temperature of reaction while being 40 ℃ system defluorinate rate be 81.2%,, when temperature of reaction is 30～40 ℃, system defluorinate rate is more or less the same, UV-US/H of the present invention 3pW 12o 4optoacoustic collaboration system has good degradation effect for PFOS, can realize simple condition and be issued to higher defluorinate rate.
Embodiment 5
High frequency US-UV/H 3pW 12o 40system is degraded in tap water medium
The tap water that processing contains PFOS, the original pH of water sample is that 7.3, PFOS concentration is 10mg/L, F -concentration is about 0 (not detecting), and turbidity is lower, does not need pre-treatment, can directly degrade.
The method of utilizing PFOS in this device degradation water, comprises the steps:
A) by pending adding in reactor 5 containing PFOS waste water, add heteropolyacid, concentration is 1g/L, PFOS/H simultaneously 3pW 12o 40(mass concentration ratio) is 1:100, adds 200mg/L H 2o 2solution, pH value is adjusted to 2 with 0.1mol/L NaOH and HCl;
B) open the power supply of ultrasonic wave 1, setting reaction power is 100W, open UV-light power supply 7 simultaneously, in reaction process, water in tank 3 relies on condensate pipe 2 to realize continuous flow, reacts, without out-source gas in air under normal pressure, temperature of reaction maintains 30 ℃ by tank 3, and system is reacted 4 hours under the condition of constant temperature;
C) close UV-light power supply 7, close ultrasonic generator 1, reaction finishes, and water outlet adopts chromatography of ions to detect F in water -concentration, determines defluorinate rate.
After testing, after reaction, the defluorinate rate of PFOS reaches 74.6%, and under same reaction conditions, UV/H 3pW 12o 40the defluorinate rate of system is 5.65%, and independent ultrasonic system defluorinate rate is 48.7%, and UV-US/H of the present invention is described 3pW 12o 4optoacoustic collaboration system has good degradation effect for PFOS in tap water medium, can realize simple condition and be issued to higher defluorinate rate.
Embodiment 6
High frequency US-UV/H 3pW 12o 40system is degraded in Natural Water medium
The Urban River Water that processing contains PFOS (Zhujiang River university city section), the original pH of water sample is that 7.03, PFOS concentration is 10mg/L, F -concentration is about 0 (not detecting), because raw water turbidity is higher, need after 0.22 μ m membrane filtration, process again.
The method of utilizing PFOS in this device degradation water, comprises the steps:
A) by pending adding in reactor 5 containing PFOS waste water, add heteropolyacid, concentration is 1g/L, PFOS/H simultaneously 3pW 12o 40(mass concentration ratio) is 1:100, adds 200mg/L H 2o 2solution, pH value is adjusted to 2 with 0.1mol/L NaOH and HCl;
B) open the power supply of ultrasonic wave 1, setting reaction power is 100W, open UV-light power supply 7 simultaneously, in reaction process, water in tank 3 relies on condensate pipe 2 to realize continuous flow, reacts, without out-source gas in air under normal pressure, temperature of reaction maintains 30 ℃ by tank 3, and system is reacted 4 hours under the condition of constant temperature;
C) close UV-light power supply 7, close ultrasonic generator 1, reaction finishes, and water outlet adopts chromatography of ions to detect F in water -concentration, determines defluorinate rate.
After testing, after reaction, the defluorinate rate of PFOS reaches 58.3%, and under same reaction conditions, UV/H 3pW 12o 40the defluorinate rate of system is 2.14%, and independent ultrasonic system defluorinate rate is 47.7%, and UV-US/H of the present invention is described 3pW 12o 4optoacoustic collaboration system still has good degradation effect for PFOS in Natural Water medium, can realize simple condition and be issued to higher defluorinate rate.
Above-described embodiment is preferably embodiment of the present invention; but embodiments of the present invention are not restricted to the described embodiments; other any do not deviate from change, the modification done under spirit of the present invention and principle, substitutes, combination, simplify; all should be equivalent substitute mode, within being included in protection scope of the present invention.

Claims (10)

1. the collaborative device that promotes the degraded of Perfluorooctane sulfonates potassium and defluorinate in water of an optoacoustic, it is characterized in that, this device comprises ultrasonic generator and is placed on ultrasonic generator for keeping the tank of temperature of reaction, in tank, be provided with the reactor containing Perfluorooctane sulfonates potassium waste water for splendid attire, described reactor top is provided with ultraviolet lamp, and this reactor is made by inertia material.
2. device according to claim 1, is characterized in that, described ultraviolet lamp is horizontally placed on reactor, and with reactor in the distance of liquid level be 3～5cm.
3. according to device described in claim 1 or 2, it is characterized in that, the power of described ultraviolet lamp is 11W, and the UV-light of transmitting 254nm.
4. install according to claim 3, it is characterized in that, described ultrasonic generator transmitting frequency is 358kHz, and rated output is 100W.
5. device according to claim 4, is characterized in that, described reactor is the cylindrical vessel being made by tetrafluoroethylene, which is provided with stopple coupon; Described tank is provided with condensate pipe.
6. the method for utilizing Perfluorooctane sulfonates potassium in the device degradation water described in claim 1～5 any one, is characterized in that, comprises the steps:
A) the pending waste water containing Perfluorooctane sulfonates potassium is added in reactor, add heteropolyacid as catalyzer, add H 2o 2as oxygenant, control pH value between 2～4;
B) open ultraviolet lamp and ultrasonic generator, it is 100W that ultrasonic power is set, and reacts 3～5 hours, gets final product water outlet.
7. method according to claim 6, is characterized in that, the mass ratio of described Perfluorooctane sulfonates potassium and heteropolyacid is 1:50～1:150, and the concentration of heteropolyacid is 0.5～1.5g/L.
8. method according to claim 6, is characterized in that, described heteropolyacid is phospho-wolframic acid.
9. method according to claim 6, is characterized in that, described reaction is carried out under the condition of 30～40 ℃ of constant temperature.
10. method according to claim 7, is characterized in that, the mass ratio of described Perfluorooctane sulfonates potassium and oxygenant is 1:5～1:20.
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CN104773884A (en) * 2015-03-11 2015-07-15 华南理工大学 Co-used iron-carbon micro-electrolysis and photo degradation two-section perfluoro octanoic acid degradation method
CN109179569A (en) * 2018-11-14 2019-01-11 四川中盛净源环保设备有限公司 A kind of processing organic wastewater with difficult degradation thereby oxidant cooperative photocatalysis oxidation reaction apparatus and application
CN110330092A (en) * 2019-06-25 2019-10-15 山东晟博生物科技有限公司 A kind of aura cracking sewage-treatment plant and sewage water treatment method
CN114502251A (en) * 2019-10-11 2022-05-13 科勒沃特科技公司 Reusable composite filter material and methods of making and using same to remove and destroy molecular contaminants in water

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