EP0808504B1 - Procede et dispositif pour traiter des huiles et solvants contamines par des substances radioactives - Google Patents

Procede et dispositif pour traiter des huiles et solvants contamines par des substances radioactives Download PDF

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Publication number
EP0808504B1
EP0808504B1 EP96904124A EP96904124A EP0808504B1 EP 0808504 B1 EP0808504 B1 EP 0808504B1 EP 96904124 A EP96904124 A EP 96904124A EP 96904124 A EP96904124 A EP 96904124A EP 0808504 B1 EP0808504 B1 EP 0808504B1
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EP
European Patent Office
Prior art keywords
water
effluent
microorganisms
oils
solvents
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP96904124A
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German (de)
English (en)
French (fr)
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EP0808504A1 (fr
Inventor
Joanes Pierre Deguitre
Maurice Stingre
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Richmond Agency Ltd
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Richmond Agency Ltd
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Publication date
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Publication of EP0808504A1 publication Critical patent/EP0808504A1/fr
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Publication of EP0808504B1 publication Critical patent/EP0808504B1/fr
Anticipated expiration legal-status Critical
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G21F9/18—Processing by biological processes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S210/00—Liquid purification or separation
    • Y10S210/902—Materials removed
    • Y10S210/911—Cumulative poison
    • Y10S210/912—Heavy metal

Definitions

  • the invention relates to a method and a device for treating oils and solvents contaminated with radioactive substances.
  • these microorganisms act in the presence of a very large amount of water and in the presence of oxygen, the ratio between respective volumes of water and oil being about 100/5 or 20/1.
  • oils and solvents contaminated by substances radioactive are subject to increasingly stringent regulations which prohibit the contamination of the atmosphere or wastewater drainage systems, in order to do not disperse the radioactive substances contained in these oils into nature and solvents.
  • the object of the present invention is to remedy the drawbacks of known methods and devices, and to provide a method and a device for treat oils and solvents contaminated with radioactive substances, this process and this device being adapted to allow discharge into the atmosphere or the networks of air and water collection, the characteristics of which comply with the requirements of regulations in force, the radioactive substances being collected in a very small volume. waste that is easy to process and store to avoid environmental contamination.
  • the process aimed by the invention for treating oils and solvents contaminated by radioactive substances comprises the step which consists in subjecting these oils and solvents to the action of micro-organisms preselected in the presence air and a very large volume of water compared to the volume of oils and solvents to be treated, these microorganisms being adapted to destroy organic molecules to transform them in particular into CO 2 and H 2 O.
  • the merit of the present inventor is that he was able, on a pilot scale, to cope with the increase in the content of treatment residues, due to the recycling of the effluents collected, so as to find himself permanently in conditions close to the initial conditions under which it is known that microorganisms are capable of degrading and breaking down oils and solvents. It is thus possible to transform the organic molecules substantially completely into CO 2 and H 2 O.
  • radioactive substances and other materials contained in the collected effluent are separated from the water in step e) and recycled or treated in step f) to constitute only a small volume of residues much easier to process and store than the initial volume of oils and solvents contaminated.
  • a volume is removed predetermined regenerated water corresponding substantially to the volume of a new load of oils and solvents contaminated with radioactive substances. This allows to check the correct operation of the operation.
  • the volume of liquid discharges from the implementation of the process according to the present invention is thus substantially equal to the volume of oils and degraded solvents, regardless of whether these liquid discharges meet completely the prescriptions of the regulations in force.
  • pre-selected mineral supports of microorganisms to fix by exchange ions at least part of the metals present in the charge.
  • a clarification of the effluent by decantation, and the sludge thus obtained is recycled to step c).
  • a evaporation of the effluent water under vacuum and the collected water is used for step g) after evaporation and condensation, while recovering the residues from this vacuum evaporation operation and subjecting them to drying in a fluidized bed.
  • the device according to the invention also comprises means, for gravity or by pumping, shown schematically at 10, to transfer to the first reactor 3 the liquid medium contained in the premixer 2, similar means shown diagrammatically in 11, to transfer the mixture leaving the first reactor 3, similar means shown diagrammatically at 12, for transferring into the clarifier 7, the mixture leaving the second reactor 5, similar means shown schematically in 13 to introduce water supernatant into a buffer tank 16 the clarifier 7, similar means 14 for recycling in the premixer 2 the sludge which accumulates at the bottom of the clarifier 7, similar means shown in 15 to send the water stored in the tank to evaporator 8 buffer 16, as well as similar means shown diagrammatically in 17, for recycling to the premixer 2 and possibly to an external network shown diagrammatically at 18, water evaporated and condensed collected in a tank 19 in which it is regenerated.
  • the means 6 for injecting air include a network, shown schematically in 20, of compressed air distribution and ramps shown diagrammatically at 21, for injecting compressed air into the lower part of the premixer 2, first reactor 3 and second reactor 5.
  • This air injection constitutes an oxygen supply in the bath of each container and ensures at the same time time for mixing said bath.
  • the first reactor 3 is equipped with a device mixer which includes a pump 22 which sends the reaction medium to the reactor 3 in a mixing tank 22a, the overflow of which, shown diagrammatically at 23, falls back into the reactor 3.
  • a device mixer which includes a pump 22 which sends the reaction medium to the reactor 3 in a mixing tank 22a, the overflow of which, shown diagrammatically at 23, falls back into the reactor 3.
  • the clarifier 7 is a clarifier of any known type that it needless to describe in detail here.
  • the clarification is carried out by decantation, the mixture coming from the second reactor 5 entering the clarifier 7 via a axial tubular column 24 and coming into contact, if necessary, with flocculation which are introduced in a manner that is not shown.
  • the residues collected at the bottom of the evaporator 8 are sent to a processing unit 25 in which they are, for example, dried and packaged for storage, since these residues include radioactive substances. If necessary, the sludge collected at the bottom of the clarifier 7 can also be sent to processing unit 25.
  • the reservoir 19 for collecting and regenerating condensed water is equipped with means known in themselves for regenerating this water.
  • the following processing device the invention is, in a preferred embodiment, installed on a platform 26 likely to be transported on the platform of a truck or trailer.
  • This platform has a peripheral side wall 27.
  • the assembly formed by the platform 26 and the wall 27 constitutes a retention tank 28 which prevents the discharge to the outside of all radioactive fluids in the event of an incident.
  • the retention tank 28 is itself covered by a substantially sealed cabin 29 maintained slightly depressed by a ventilation and air filtering system 30, of a any known type that need not be described here.
  • the method implemented in the device 1 according to the invention for treating oils and solvents contaminated by radioactive substances, comprises the conventional step which consists in subjecting these oils and solvents to the action of micro-organisms preselected in the presence air and a very large volume of water compared to the volume of oils and solvents to be treated, these microorganisms being adapted to destroy organic molecules to transform them in particular into CO 2 and H 2 O.
  • This process was developed to treat oils and solvents contaminated with radio elements and produced by mechanical maintenance activities equipment located in controlled areas of nuclear power plants and other facilities and nuclear reactors.
  • oils and solvents which are stored in containers, are radioactive and contaminated in particular by long-lived radio-elements following: cobalt 58, 60 and 62, manganese 54, silver 110, cesium 134 and 137, zinc 65, niobium 95, antimony 124 and 125.
  • the average activity rate of contaminated products is around 700 Becquerels per liter, with varying rates depending on the container, from 50 to 9,000 Becquerels per liter.
  • Oils and solvents are composed, more than 98%, of an apolar fraction essentially containing saturated hydrocarbons C n H 2n + 2, with a predominance of alkanes nC 20 and nC 21 which correspond to branched aliphatic hydrocarbons.
  • the merit of the present inventor has been to solve this problem of gelling whose formation from metabolites may be faster than degradation of these same metabolites, by developing a method allowing avoid this gelation.
  • the most important and representative mechanism is the degradation of alkanes by oxidation of the methyl terminal group.
  • the carbon of the terminal methyl group -CH 3 is oxidized to primary alcohol -CH 2 OH, then to aldehyde-CHO then to primary acid -CH 2 OH. This acid is then metabolized by ⁇ -oxidation directly or via the formation of diacid ( ⁇ -hydroxylation).
  • the oxidation of the methyl group is considered the main metabolic pathway.
  • the mechanism oxidation of the methyl group is no different from the oxidation mechanism of n-alkanes.
  • polyethylene glycol gives compounds which, according to the number of monomers, can be liquid or solid and the mixture of which can give a viscous product close to gelation.
  • the free water produced represents approximately 80% of the weight oils and solvents treated if natural evaporation is not taken into account and of the addition of water necessary for the seeding and life of microorganisms (development and reproduction).
  • the temperature, 30 to 35 ° C, and the pH, from 6.5 to 7.5, have the values recommended for the development and action of microorganisms.
  • microorganisms are chosen from microorganisms industrial products available on the market. They are for example chosen from the range "BIO ACTIV 200" from TBA (TECHNIQUES AND BIOCHEMISTRY) APPLIED). These microorganisms can be conventionally attached to mineral carriers and are conventionally used with nutrients suitable, as well as with emulsifying agents.
  • microorganisms used are therefore mixtures of strains known and substantially specialized in attacking specific products. These mixtures are conventionally prepared to be effective for decompose the main constituents of the oils and solvents to be degraded, but also the aforementioned intermediate by-products of decomposition of these constituents.
  • the nutritional balance of the bath must be constantly maintained in the report CARBON / NITROGEN / PHOSPHORUS little different from 100/5/1.
  • the contents of the reaction bath in microorganisms and nutrients are the usual ones for these materials.
  • pre-selected digital media are used on which are fixed the micro-organisms and which will fix by ion exchange the radioactive heavy metals present in the charge.
  • microorganisms without supports minerals and available in solutions.
  • the mixture is clarified coming from the second reactor 5 by decantation, adding, if necessary, a flocculant which does not interfere with the smooth running of the process, and the sludge is recycled thus obtained towards step c).
  • Evaporation of the effluent from the water is carried out under vacuum.
  • the clarification and the water collected after evaporation is used for step g) and condensation.
  • This regeneration can be done for example by adding peroxide hydrogen and soda.
  • waste includes the two aforementioned by-products as well as polyethylene glycol.
  • the proportion of this waste is around 3 per thousand by weight: this means that we will find around 3Kg of final waste for around 1000 Kg degraded oils or solvents.
  • the device according to the invention which is in the form of an installation mounted on at least one platform transportable by road, can be easily moved from one site to another to treat in each site the contaminated oils and solvents and decompose them essentially into CO 2 and H 2 O, with a very low quantity of releases containing radioactive substances, of the order of 3 per thousand by weight of the oils and solvents treated.
  • This device also has the advantage of eliminating any transport of radioactive oils and solvents to a site for processing these oils and solvents.
  • the mixture resulting from biodegradation in reactor 3 is transferred by the pump 37 into a primary decanter 41 at a rate largely higher than the nominal installation flow.
  • the biomass recovered from the bottom of the primary settling tank 41 is returned in the premixer 2 by the pump 14.
  • the mixture thus freed from most of the materials suspension and incompletely degraded fat is transferred to the reactor 5 by means of pump 11.
  • the COD at this time is of the order of 40,000 ppm.
  • the mixture thus transferred to reactor 5 is again subjected to the action of new microorganisms that destroy fatty acids. This done drop the COD to a rate close to 300 ppm.
  • the mixture treated in reactor 5 is sent by means of the pump 54 in the clarifier 7 at a flow slightly higher than the nominal flow so that on the other hand, the last fatty elements which could have escaped the action of micro-organisms, pour into a recovery tank 52 from where they are taken up by means of the pump 12 to be sent to the premixer 2.
  • Clarified water which contains some miscible products, biodegradation byproducts such as Diethylene glycol dibutyl ether, Polyethylene glycol Methyl Ether and Ditertiobuthyl-4-methyl phenol plus residues of carbon chains (n-alkanes C 11 to C 21 ), is sent to the vacuum evaporator 8.
  • biodegradation byproducts such as Diethylene glycol dibutyl ether, Polyethylene glycol Methyl Ether and Ditertiobuthyl-4-methyl phenol plus residues of carbon chains (n-alkanes C 11 to C 21 ).
  • the demineralized water produced by the condenser 9 of the evaporator 8 is sent to container 19 where it is regenerated by means of system 40 in REDOX potential with hydrogen peroxide, pH with soda and aerated by forced recirculation through a microporous sprayer.
  • This water as well reconstituted with the characteristics of industrial water is returned to the premixer 2 where it participates in a new degradation cycle.
  • Such treatment is known in itself.
  • the condenser 9 is associated with a group of classic 9a refrigeration.
  • the ultimate waste recovered at the bottom of the evaporator 8 is sent to a buffer tank 24 whose volume corresponds to three days of walking the installation.
  • the product is homogenized by adding water and air, then it is sent under pressure through an atomizer in the drying unit 25 in bed fluidized.
  • Activated carbon filter virtually eliminates the last materials organic matter contained in this regenerated condensed water.
  • a reservoir 60 is used to reactivate and develop microorganisms and nutrients that are fed by three metering devices 61a, 61b, 61c.
  • Three feeders 62a, 62b, 62c with adjustable flow are intended to supply micro-organisms to the premixer 2 and to the reactors 3 and 5. It a supply 63 of air or oxygen is provided.
  • the water taken from premixer 2 arrives at 64. It is kept at the temperature of 35 ° C by means of a circulating fluid heater operating in such a way that microorganisms never pass into the circulating fluid heater, the internal temperature of which would be fatal to microorganisms.
  • the distributor with three compartments 61a, 61b, 61c, sends microorganisms, trace elements and nutrients.
  • Microorganisms wake up, then develop to form a biomass whose composition will be thousands of times greater than that which found in the installation, thereby increasing the speed of degradation of the chains carbon, resulting COD.
  • This preparation method allows increase the capacity of the processing unit by around 50%.
  • the hydro-ejector 66 represented in FIG. 5, of conventional structure, includes a centrifugal pump, not shown, feeding a calibrated nozzle 67 located in the center and in the axis of an annular chamber 68, an air / water mixing tube 69 and a diffuser 70.
  • the assembly is completed by an air inlet pipe atmospheric, an oximeter and a valve for regulating the water supply (not represented).
EP96904124A 1995-02-10 1996-02-12 Procede et dispositif pour traiter des huiles et solvants contamines par des substances radioactives Expired - Lifetime EP0808504B1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
FR9501581 1995-02-10
FR9501581A FR2730584B1 (fr) 1995-02-10 1995-02-10 Procede et dispositif pour traiter des huiles et solvants contamines par des substances radioactives
PCT/FR1996/000225 WO1996024937A1 (fr) 1995-02-10 1996-02-12 Procede et dispositif pour traiter des huiles et solvants contamines par des substances radioactives

Publications (2)

Publication Number Publication Date
EP0808504A1 EP0808504A1 (fr) 1997-11-26
EP0808504B1 true EP0808504B1 (fr) 1999-05-19

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EP96904124A Expired - Lifetime EP0808504B1 (fr) 1995-02-10 1996-02-12 Procede et dispositif pour traiter des huiles et solvants contamines par des substances radioactives

Country Status (19)

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US (1) US5948259A (zh)
EP (1) EP0808504B1 (zh)
JP (1) JP3256240B2 (zh)
KR (1) KR100301228B1 (zh)
CN (1) CN1173946A (zh)
AU (1) AU4833896A (zh)
BG (1) BG63354B1 (zh)
BR (1) BR9607727A (zh)
CA (1) CA2211104C (zh)
CZ (1) CZ293133B6 (zh)
DE (1) DE69602520T2 (zh)
EA (1) EA000170B1 (zh)
ES (1) ES2134593T3 (zh)
FI (1) FI973070A (zh)
FR (1) FR2730584B1 (zh)
HU (1) HUP9801212A3 (zh)
SK (1) SK283180B6 (zh)
UA (1) UA41438C2 (zh)
WO (1) WO1996024937A1 (zh)

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US7037403B1 (en) * 1992-12-28 2006-05-02 Applied Materials Inc. In-situ real-time monitoring technique and apparatus for detection of thin films during chemical/mechanical polishing planarization
JP3736165B2 (ja) * 1998-12-28 2006-01-18 株式会社日立製作所 界面活性剤を含む放射性廃液の処理方法及びその処理装置
ES2190758B8 (es) * 2002-01-02 2014-06-05 Universidad Politécnica de Madrid Procedimiento de biorremediación para la concentración y eliminación de radionúclidos en las aguas radiactivas de las piscinas nucleares.
BRPI0511684B1 (pt) 2004-05-30 2017-06-20 Pebble Bed Modular Reactor Proprietary Method of treatment of irradiated material
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JP4631007B2 (ja) * 2005-09-09 2011-02-16 独立行政法人 日本原子力研究開発機構 微生物による有機系液体廃棄物の分解・処理方法
KR100837177B1 (ko) * 2007-11-30 2008-06-11 권오경 방사성 폐기물 건조기
JP4774120B2 (ja) * 2008-02-08 2011-09-14 三菱重工業株式会社 放射性硝酸塩廃液処理装置及び方法
KR100884004B1 (ko) * 2008-08-18 2009-02-17 테크밸리 주식회사 폐 방사능 유기용매 처리장치
FR2937646B1 (fr) * 2008-10-27 2011-07-29 Dewdrops Procede et dispositif de traitement par voie biologique d'une charge liquide contaminee comprenant une phase liquide organique dispersible et digestible telle qu'une huile ou solvant toxique
FR2963846B1 (fr) * 2010-08-13 2012-08-17 Dominique Deguitre Procede et dispositif pour traiter des huiles, graisses, solvants, eaux ou boues huileuses contamines par des radionucleides
KR101306052B1 (ko) * 2011-05-17 2013-09-09 한국수력원자력 주식회사 방사성 폐유 처리장치 및 이를 이용한 방사성 폐유 처리방법
US9896351B2 (en) * 2013-03-15 2018-02-20 Avantech, Inc. Method for removal of radionuclides in liquids
CN108565037B (zh) * 2018-03-23 2020-10-27 岭东核电有限公司 压水堆核电厂放射性废油的催化再生方法
CN108511100B (zh) * 2018-03-23 2019-11-05 岭东核电有限公司 压水堆核电厂放射性废油的处理方法
CN108428485B (zh) * 2018-03-23 2019-09-17 岭东核电有限公司 百万千瓦级核电厂放射性废油的再生方法
CN108597637B (zh) * 2018-03-23 2020-10-27 岭东核电有限公司 百万千瓦级核电厂放射性废油的处理方法

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Also Published As

Publication number Publication date
ES2134593T3 (es) 1999-10-01
MX9706099A (es) 1997-10-31
EA199700094A1 (ru) 1998-02-26
AU4833896A (en) 1996-08-27
HUP9801212A2 (hu) 1998-09-28
FI973070A0 (fi) 1997-07-18
KR100301228B1 (ko) 2001-09-03
DE69602520T2 (de) 1999-10-07
CA2211104C (en) 2001-10-09
CN1173946A (zh) 1998-02-18
CZ243297A3 (cs) 1998-01-14
CZ293133B6 (cs) 2004-02-18
BG101819A (en) 1998-07-31
US5948259A (en) 1999-09-07
BG63354B1 (bg) 2001-10-31
EA000170B1 (ru) 1998-10-29
JP3256240B2 (ja) 2002-02-12
FI973070A (fi) 1997-10-10
WO1996024937A1 (fr) 1996-08-15
DE69602520D1 (de) 1999-06-24
SK283180B6 (sk) 2003-03-04
FR2730584A1 (fr) 1996-08-14
BR9607727A (pt) 1998-07-14
SK104497A3 (en) 1998-03-04
JP2000515622A (ja) 2000-11-21
FR2730584B1 (fr) 1997-04-25
CA2211104A1 (en) 1996-08-15
KR19980702096A (ko) 1998-07-15
HUP9801212A3 (en) 2001-10-29
UA41438C2 (uk) 2001-09-17
EP0808504A1 (fr) 1997-11-26

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