EP1453938B1 - Verfahren zur zerstörung von nuklearem graphit durch vergasung in wässrigem medium - Google Patents

Verfahren zur zerstörung von nuklearem graphit durch vergasung in wässrigem medium Download PDF

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Publication number
EP1453938B1
EP1453938B1 EP02799804A EP02799804A EP1453938B1 EP 1453938 B1 EP1453938 B1 EP 1453938B1 EP 02799804 A EP02799804 A EP 02799804A EP 02799804 A EP02799804 A EP 02799804A EP 1453938 B1 EP1453938 B1 EP 1453938B1
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EP
European Patent Office
Prior art keywords
graphite
process according
treatment process
voltage pulses
carbon
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
EP02799804A
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English (en)
French (fr)
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EP1453938A2 (de
Inventor
Jacques Paris
Jean-Raymond Costes
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.)
Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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Commissariat a lEnergie Atomique CEA
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Publication of EP1453938B1 publication Critical patent/EP1453938B1/de
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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72—Other features
    • C10J3/723—Controlling or regulating the gasification process
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B02—CRUSHING, PULVERISING, OR DISINTEGRATING; PREPARATORY TREATMENT OF GRAIN FOR MILLING
    • B02C—CRUSHING, PULVERISING, OR DISINTEGRATING IN GENERAL; MILLING GRAIN
    • B02C19/00—Other disintegrating devices or methods
    • B02C19/18—Use of auxiliary physical effects, e.g. ultrasonic waves or irradiation, for disintegrating
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/02—Fixed-bed gasification of lump fuel
    • C10J3/06—Continuous processes
    • C10J3/18—Continuous processes using electricity
    • 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
    • G21F9/28—Treating solids
    • G21F9/30—Processing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B02—CRUSHING, PULVERISING, OR DISINTEGRATING; PREPARATORY TREATMENT OF GRAIN FOR MILLING
    • B02C—CRUSHING, PULVERISING, OR DISINTEGRATING IN GENERAL; MILLING GRAIN
    • B02C19/00—Other disintegrating devices or methods
    • B02C19/18—Use of auxiliary physical effects, e.g. ultrasonic waves or irradiation, for disintegrating
    • B02C2019/183—Crushing by discharge of high electrical energy
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2200/00—Details of gasification apparatus
    • C10J2200/12—Electrodes present in the gasifier
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2200/00—Details of gasification apparatus
    • C10J2200/33—Laboratory scale gasifiers
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens

Definitions

  • the present invention relates to a method of destruction of a nuclear graphite contaminated by radioelements by gasification of said graphite aqueous medium.
  • the general area is therefore the treatment nuclear waste, such as graphite from the natural uranium-graphite-gas sector (known as UNGG), recovered during the dismantling of said die.
  • UNGG natural uranium-graphite-gas sector
  • waste treatment such as nuclear graphite contaminated with radioelements
  • waste treatment is done either by storing all the waste in appropriate containers, either by destruction total waste by combustion.
  • waste is ground in a first step according to a mechanical grinding process, in a chamber of confinement, so as to obtain a size of particles weak enough to be able then constitute a fluidized bed or suspension in fuel and perform particle combustion as well produced.
  • the object of the present invention is to propose a contaminated nuclear graphite treatment process by radioelements to counteract aforementioned disadvantages of the prior art.
  • the subject of the invention is a process for treating a nuclear graphite contaminated with radioelements, said method comprising a step of subjecting said graphite, placed in immersion in a medium containing water, to high voltage pulses, said pulses having a sufficient energy for electric arcs to trigger and break the links constituents of water molecules and carbon-carbon of said graphite, the number of pulses high voltage being determined so as to obtain a transformation in the form of gas of said graphite.
  • High voltage pulses electrical impulses may carry a voltage of the order of one to several kilovolts, so as to obtain an arc in the medium containing water. Over there next, we will reason in terms of electrical energy, the latter being at the origin of the creation of arcs responsible for their interaction with the aqueous medium and the conductive carbonaceous material of the gasification of said material.
  • E represents the electrical energy conveyed by a high voltage pulse or more precisely the energy of electric arcs.
  • -C represents an atom of carbon taken in a carbon-carbon bond.
  • this method makes it possible to obtain a destruction of nuclear graphite, radioelements remaining trapped in the medium containing water.
  • this process advantageously makes it possible to obtain the production of gas, said gases being recoverable and reused for various applications.
  • the person skilled in the art can choose the application conditions of high voltage pulses (energy, frequency, duration and number of pulses sent) depending on the nature of the graphite treat, with the understanding that the higher the energy of impulses will be important plus the number of impulses to apply will be less, to obtain the said gasification.
  • the energy of the pulses voltage can be 100 J to 100 kJ.
  • Such a value of energy pulses allows, at each pulse, to generate, advantageously, the rupture of a large number of water molecules and carbon-carbon bonds constituent of the graphite to be treated.
  • the high voltage pulses may have a duration ranging from 200 ns at 100 ⁇ s with preferably a duration of 1 ⁇ s.
  • the high voltage pulses can have a frequency ranging from 1 to 1000 Hz, preferably 10 Hz.
  • the medium containing water may contain, advantageously, according to the invention, at least one radical stabilization catalyst, allowing the stabilization of the radicals formed above.
  • the treatment method of nuclear graphite may advantageously comprise a step of evacuating said gases produced with a view to the use of the gases produced.
  • This step presents the advantage of avoiding any phenomenon of overpressure inherent in the production of gas in a closed environment and to deliver the gases produced either to a place of storage, or to a place of treatment.
  • the gas evacuation step is carried out by continuous scanning of the surface of the medium containing water with an inert gas, preferably with nitrogen.
  • the treatment method of graphite comprises preferably, after gasification of the graphite, a step treatment of the medium containing water.
  • This treatment can correspond to conventional treatment liquid effluents intended to recover and reconcentrate, for example, the heavy metals contained initially in the graphite to be processed and released in the aqueous medium after gasification of graphite.
  • This treatment may also be intended to clean up the medium containing water, in which took place the gasification of graphite, released radioelements by graphite.
  • radioactive cesium in the form of ionic in water can be trapped by means of resins ion exchangers or calixarenes.
  • Cobalt under form of oxides, can be filtered.
  • Tritium as he is fixed on water instead of hydrogen by isotopic exchange and can then be concentrated for deactivation.
  • Figure 1 illustrates a particular device to implement the invention.
  • Figure 2 shows curves illustrating the % rate of gas produced according to the number of high voltage pulses n, these curves coming from of an experiment using the device of the figure 1.
  • Figure 3 illustrates another type of device particular for implementing the invention.
  • the process according to the invention consists in treating the nuclear graphite contaminated with radioelements, by sending on said graphite of high voltage pulses in aqueous medium.
  • FIG. 1 illustrates such a device allowing to proceed to the treatment of such a type of graphite.
  • This device comprises a sealed and non-metallic reactor 1, for example made of polyethylene.
  • the bottom of the reactor is a conductive plate, constituting the earth electrode 2, connected to a high voltage generator 3, of the Marx generator type, said generator supplying a high voltage electrode 4, the distance of which can be adjusted. vis-à-vis the earth electrode 2, in order to adjust the potential difference applied between these two electrodes.
  • a nuclear graphite block 5 Between the electrodes 2 and 4 is placed a nuclear graphite block 5, said block being totally immersed in water 6. This device makes it possible to emit high voltage pulses in the direction of the block.
  • the pulses thus emitted of given energy cause the appearance of an electric arc between the electrodes which, in its way, dissociates the water in free radicals and breaks carbon-carbon bonds in contact with the graphite, to form carbon radicals .
  • the chemical reaction between the carbon atoms in the form of radicals and the radicals resulting from the decomposition of water lead to the formation of CO, CO 2 and H 2 .
  • the gases 7 produced are conveyed via a pump 8 to a gas detector 9 comprising means for detecting carbon monoxide 10, carbon dioxide 11, oxygen 12 and methane 13. Once passed through the detector 9, the gases produced are routed back to the reactor 1.
  • a gasometer system 14 is provided to measure the production of gas and avoid any overpressure.
  • a system intended to ensure the regeneration of the aqueous medium, in order to maintain the qualities of that medium necessary to the formation of electric arcs, can be considered.
  • Figure 2 shows the% carbon monoxide and carbon dioxide levels recorded as a function of the number of pulses applied n. It can be seen that the CO ratio, represented on the CO curve, and the CO 2 content , represented on the CO 2 curve, increase with the number of pulses until reaching a plateau shape, from 220 shots according to the conditions of realization of this example.
  • Figure 3 illustrates a device for implementing the invention with, in this case, a continuous scan with an inert gas.
  • This figure proposes a device similar to the preceding, except that the reactor 1 is fed with a continuous and constant flow of inert gas, such as N 2 , by means of a bottle 18 provided with a manometer.
  • the gases produced are always routed to a detection device 9 provided with means for detecting carbon monoxide 10, carbon dioxide 11, oxygen 12 and methane 13 by means of a pump 8, the whole being connected a data processing system 20, which will allow, in particular, to produce curves, highlighting the rate of gas produced at a given time, since the gases do not stagnate in the reactor.
  • a flow meter 19 measures the flow rate of the total gases, which are rejected. This last device is easier to manage because it avoids the accumulation of gases and the possibility of existence of explosive mixtures.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Organic Chemistry (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Health & Medical Sciences (AREA)
  • High Energy & Nuclear Physics (AREA)
  • General Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Toxicology (AREA)
  • Food Science & Technology (AREA)
  • Carbon And Carbon Compounds (AREA)
  • Processing Of Solid Wastes (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)

Claims (9)

  1. Verfahren zur Behandlung eines Reaktorgraphits, der durch Radioelemente kontaminiert ist, das eine Stufe umfasst, bei welcher der Graphit, der in ein Wasser enthaltendes Medium eingetaucht ist, Hochspannungsimpulsen ausgesetzt wird, die eine ausreichende Energie aufweisen, um elektrische Lichtbögen auszulösen und einen Bruch der Bindungen der Wassermoleküle und der Kohlenstoff-Kohlenstoff-Bindungen des Graphits zu bewirken, wobei die Anzahl der Hochspannungsimpulse so festgelegt wird, dass eine Umwandlung in gasförmigen Graphit erzielt wird
  2. Verfahren nach Anspruch 1, bei dem die Energie der Hochspannungsimpulse 100 J bis 100 kJ beträgt.
  3. Verfahren nach einem der Ansprüche 1 oder 2, bei dem die Hochspannungsimpulse eine Dauer von 200 ns bis 100 µs haben.
  4. Verfahren nach einem der vorhergehenden Ansprüche, bei dem die Hochspannungsimpulse eine Frequenz von 1 bis 1000 Hz haben.
  5. Verfahren nach einem der Ansprüche 1 bis 4, bei dem das Wasser enthaltende Medium mindestens einen Katalysator zur Stabilisierung von Radikalen enthält.
  6. Verfahren nach einem der vorhergehenden Ansprüche, das eine Stufe des Abzugs der gebildeten Gase zur Verwendung der gebildeten Gase umfasst.
  7. Verfahren nach Anspruch 6, bei dem die Stufe des Abzugs der Gase durch kontinuierliche Spülung mit einem inerten Gas erfolgt.
  8. Verfahren nach Anspruch 7, bei dem das inerte Gas Stickstoff ist.
  9. Verfahren nach einem der Ansprüche 1 bis 8, das eine Stufe zur Behandlung des Wasser enthaltenden Mediums umfasst.
EP02799804A 2001-12-11 2002-12-10 Verfahren zur zerstörung von nuklearem graphit durch vergasung in wässrigem medium Expired - Lifetime EP1453938B1 (de)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
FR0115974A FR2833269B1 (fr) 2001-12-11 2001-12-11 Procede de gazeification d'une matiere carbonee conductrice par application d'impulsions haute tension a ladite matiere en milieu aqueux
FR0115974 2001-12-11
PCT/FR2002/004253 WO2003050208A2 (fr) 2001-12-11 2002-12-10 Procede de destruction d'un graphite nucleaire par gazeification en milieu aqueux

Publications (2)

Publication Number Publication Date
EP1453938A2 EP1453938A2 (de) 2004-09-08
EP1453938B1 true EP1453938B1 (de) 2005-05-25

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EP02799804A Expired - Lifetime EP1453938B1 (de) 2001-12-11 2002-12-10 Verfahren zur zerstörung von nuklearem graphit durch vergasung in wässrigem medium

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US (1) US7465377B2 (de)
EP (1) EP1453938B1 (de)
JP (1) JP4272527B2 (de)
AT (1) ATE296339T1 (de)
DE (1) DE60204351T2 (de)
ES (1) ES2242095T3 (de)
FR (1) FR2833269B1 (de)
WO (1) WO2003050208A2 (de)

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FR2833192B1 (fr) 2001-12-11 2004-08-06 Commissariat Energie Atomique Procede de broyage d'une matiere carbonee conductrice par application d'impulsions haute-tension en milieu liquide
KR100724710B1 (ko) * 2002-11-21 2007-06-04 가부시끼가이샤 도시바 방사화 부품의 화학적 오염제거 시스템 및 방법
FR2874023B1 (fr) * 2004-08-04 2007-06-08 Commissariat Energie Atomique Procede de fabrication d'un gaz combustible par action d'un plasma immerge sur de la matiere organique en milieu aqueux
US8740873B2 (en) * 2007-03-15 2014-06-03 Hologic, Inc. Soft body catheter with low friction lumen
ATE537903T1 (de) 2007-03-16 2012-01-15 Selfrag Ag Anordnung zur elektrodynamischen fragmentierung von proben
FR2934079A1 (fr) * 2008-07-17 2010-01-22 Arbresle Ingenierie Procede d'elimination des dechets radioactifs solides a faible ou moyenne activite et vie longue par injection a grande profondeur apres transformation en emulsion aqueuse.
FR2942149B1 (fr) * 2009-02-13 2012-07-06 Camille Cie D Assistance Miniere Et Ind Procede et systeme de valorisation de materiaux et/ou produits par puissance pulsee
US20150025294A1 (en) * 2012-02-14 2015-01-22 Ald Vaccum Technologies Gmbh Decontamination Method for Radioactively Contaminated Material
FI126167B (en) * 2012-10-31 2016-07-29 Teknologian Tutkimuskeskus Vtt Oy Method for treatment of waste material and use of gaseous material
US9170193B2 (en) 2013-06-06 2015-10-27 General Electric Company Detecting coolant leaks in turbine generators
US9097657B2 (en) 2013-07-23 2015-08-04 General Electric Company Leak detection of stator liquid cooling system
JP6947126B2 (ja) * 2018-06-12 2021-10-13 株式会社Sumco シリコンロッドの破砕方法及び装置並びにシリコン塊の製造方法
CN110215985B (zh) * 2019-07-05 2021-06-01 东北大学 一种用于矿石粉碎预处理的高压电脉冲装置

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Also Published As

Publication number Publication date
US7465377B2 (en) 2008-12-16
FR2833269B1 (fr) 2004-10-15
JP4272527B2 (ja) 2009-06-03
WO2003050208A2 (fr) 2003-06-19
ATE296339T1 (de) 2005-06-15
JP2005512073A (ja) 2005-04-28
ES2242095T3 (es) 2005-11-01
US20050124842A1 (en) 2005-06-09
DE60204351D1 (de) 2005-06-30
FR2833269A1 (fr) 2003-06-13
DE60204351T2 (de) 2006-01-26
WO2003050208A3 (fr) 2004-02-12
EP1453938A2 (de) 2004-09-08

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