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EP0156001B1 - Process for conditioning contaminated waste by coating with cement - Google Patents

Process for conditioning contaminated waste by coating with cement Download PDF

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Publication number
EP0156001B1
EP0156001B1 EP84114497A EP84114497A EP0156001B1 EP 0156001 B1 EP0156001 B1 EP 0156001B1 EP 84114497 A EP84114497 A EP 84114497A EP 84114497 A EP84114497 A EP 84114497A EP 0156001 B1 EP0156001 B1 EP 0156001B1
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EP
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Prior art keywords
waste
cement
mixture
water
dry
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
Application number
EP84114497A
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German (de)
French (fr)
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EP0156001A3 (en
EP0156001A2 (en
Inventor
Heinz Mallek
Egon Dr. Zange
Wolfgang Schlenter
Karl Trümper
Siegfried Meininger
Dietmar Bege
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.)
Forschungszentrum Juelich GmbH
Siemens AG
Original Assignee
Forschungszentrum Juelich GmbH
Kernforschungsanlage Juelich GmbH
Kraftwerk Union AG
Siemens AG
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Priority to AT84114497T priority Critical patent/ATE41553T1/en
Publication of EP0156001A2 publication Critical patent/EP0156001A2/en
Publication of EP0156001A3 publication Critical patent/EP0156001A3/en
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Publication of EP0156001B1 publication Critical patent/EP0156001B1/en
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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
    • G21F9/28—Treating solids
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • G21F9/304—Cement or cement-like matrix

Definitions

  • the invention relates to a method for conditioning contaminated waste by cementing.
  • Dry waste is cemented, in particular waste that is obtained as ash after burning combustible waste or as a dry residue in the processing of sludge.
  • Radioactive waste can be included by cementing. Toxic waste that cannot be processed further and cannot be deposited directly because of its solubility in water can be stored in this way.
  • contaminated waste used here includes such substances and other comparable harmful waste that has to be stored.
  • the leaching behavior of the mixture after the cement has set and hardened when it comes into contact with water is of crucial importance.
  • the lowest possible leaching rate of the mixture body is aimed at, so that in the event of an accident in the deposit associated with water ingress, contaminated waste enclosed in the mixture body cannot escape into the water.
  • the strength of the mixture body in particular its compressive strength and surface hardness, must not be less than a minimum in order to avoid abrasion and thus the release of contaminated waste into the environment.
  • the leaching behavior of the mixture body depends strongly on its porosity.
  • the strength of the mixture body is also influenced by the porosity.
  • the highest possible material density should therefore be aimed for. It is also important to keep the volume to be brought into deposits for depositing the contaminated waste as low as possible, since the space available for deposit is not available in natural soil, for example in salt deposits.
  • the object of the invention is to provide a method for conditioning dry contaminated waste which enables a high concentration of waste in the end product with at least the same leaching behavior.
  • the strength of the set and hardened mixture body in particular its compressive strength, surface hardness and abrasion resistance, is to be improved.
  • An advantage of the setting of the waste / cement mixture under pressure is also that under these conditions a pre-sorting of the waste into waste ash, slag, and scrap can be omitted.
  • the flowable portions of the waste / cement mixture also fill tight cavities under pressure.
  • the compressed mixture has a small volume.
  • the waste / cement mixture is preferably mixed with water in a water: cement ratio in the range from 0.29 to 0.35: 1.
  • the stoichiometric water / cement ratio required to set the cement is decisive for the lower limit.
  • the upper limit is determined by the compressibility of the mixture, because with increasing water content the porosity of the set mixture increases.
  • the water content should be such that no free water is squeezed out of the mixture under pressure.
  • a ratio of 0.3: 1 has been found to be optimal for the water: cement ratio, even at high pressures, claim 3.
  • a sufficient compression of the waste / cement mixture requires at least a pressure of approx. 5 MPa corresponding to 51 kp / cm 2 .
  • the compaction of the waste / cement mixture increases disproportionately with higher pressure: with compaction with a pressure that is 8.5 times higher, about 1.2 times.
  • the compressed mixture is set without pressure.
  • Dry radioactive ash accumulated in a combustion furnace in the present heterogeneous structure was mixed with Portland cement in the ash: cement weight ratio of 2: 1 as waste.
  • this mixture was water in a water: cement ratio of 0.3: 1 admitted.
  • the dry waste content in the mixture to be set was therefore about 60% by weight.
  • the mass ratios of waste: cement were approximately 0.65: 1 and water: cement - 0.4: 1.
  • the mixture thus contained only about 30% by weight of dry waste.
  • the table below shows the densities in g / cm 3 obtained by applying increasing pressure p in MPa [or kp / cm 2 ] after the mixture has set and hardened.
  • a pressure of at least 7 MPa is therefore preferably used, claim 4.
  • the reduction in volume during the transition from the raw ash into the pressed mixture consisting of ash, cement and water was considerable.
  • the volume was reduced by a factor of 2.7; in the unpressurized process, this factor is close to 1.

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  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Processing Of Solid Wastes (AREA)
  • Treatment Of Sludge (AREA)

Abstract

A process for the conditioning of contaminated waste through cementing. Dry waste is cemented, especially waste which is recovered as ashes subsequent to the combustion of burnable waste, or as a dry residue during the treatment of sludge. In the process there is added to the dry waste a cement component not less than about 50% by weight of the weight of the waste, wherein subsequent to the admixing of the waste with the cement, there is mixed in water to the cement in a slightly excess stoichiometric ratio of effecting the setting, and the mixture is compacted under pressure and then encased.

Description

Die Erfindung bezieht sich auf ein Verfahren zum Konditionieren kontaminierten Abfalls durch Zementieren. Es wird trockener Abfall zementiert, insbesondere Abfall, der als Asche nach Verbrennung brennbaren Abfalls oder als Trockenrückstand bei der Aufarbeitung von Schlamm gewonnen ist.The invention relates to a method for conditioning contaminated waste by cementing. Dry waste is cemented, in particular waste that is obtained as ash after burning combustible waste or as a dry residue in the processing of sludge.

Es ist bekannt, schwach- bis mittelradioaktive Abfallstoffe, die brennbare Anteile enthalten, in Verbrennungsöfen zu veraschen und radioaktive Flüssigkeiten durch Eindampfen zu konzentrieren und den erhaltenen Schlamm zu Trockenrückstand zu verarbeiten. Da die Radioaktivität von schwach- bis mittelradioaktiven Abfallstoffen erst in längerer Zeit abklingt, ist es üblich, die trockenen Abfälle mit Bitumen oder Zement zu versetzen und sie in Metallfässer einzusetzen. Der Anteil des trockenen Abfalls in solchen Zementfässern beträgt etwa 25 Gew.%.It is known to incinerate low- to medium-level radioactive waste containing combustible components in incinerators and to concentrate radioactive liquids by evaporation and to process the sludge obtained into dry residue. Since the radioactivity of weakly to moderately radioactive waste materials decays only over a long period of time, it is customary to add dry bitumen or cement to the dry waste and use it in metal drums. The proportion of dry waste in such cement drums is about 25% by weight.

Es lassen sich nicht nur radioaktive Abfallstoffe durch Zementieren einschließen. Auch toxischer Abfall, der sich nicht weiterverarbeiten läßt und wegen seiner Löslichkeit in Wasser nicht unmittelbar deponierfähig ist, ist auf diese Weise lagerbar. Die hier verwendete Bezeichnung « kontaminierter Abfall schließt solche Stoffe und anderen damit vergleichbaren schädlichen Abfall, der zu lagern ist, ein.Not only radioactive waste can be included by cementing. Toxic waste that cannot be processed further and cannot be deposited directly because of its solubility in water can be stored in this way. The term “contaminated waste” used here includes such substances and other comparable harmful waste that has to be stored.

Beim Zementieren kontaminierten Abfalls ist einerseits das Auslaugverhalten des nach Abbinden und Aushärten des Zements entstandenen Gemischkörpers bei dessen Kontakt mit Wasser, andererseits dessen Festigkeit von entscheidender Bedeutung. Es wird eine möglichst geringe Auslaugrate des Gemischkörpers angestrebt, damit im Falle eines mit Wassereinbruch verbundenen Störfalls in der Lagerstätte kein im Gemischkörper eingeschlossener kontaminierter Abfall in das Wasser austreten kann. Aber auch die Festigkeit des Gemischkörpers, insbesondere dessen Druckfestigkeit und Oberflächenhärte, darf ein Mindestmaß nicht unterschreiten, um Abrieb und damit Freisetzung kontaminierten Abfalls in die Umgebung zu vermeiden.When cementing contaminated waste, the leaching behavior of the mixture after the cement has set and hardened when it comes into contact with water is of crucial importance. The lowest possible leaching rate of the mixture body is aimed at, so that in the event of an accident in the deposit associated with water ingress, contaminated waste enclosed in the mixture body cannot escape into the water. However, the strength of the mixture body, in particular its compressive strength and surface hardness, must not be less than a minimum in order to avoid abrasion and thus the release of contaminated waste into the environment.

Das Auslaugverhalten des Gemischkörpers hängt stark von dessen Porosität ab. Von der Porosität wird auch die Festigkeit des Gemischkörpers beeinflußt. Es ist deshalb eine möglichst hohe Materialdichte anzustreben. Auch kommt es darauf an, das in Lagerstätten einzubringende Volumen zur Ablagerung der kontaminierten Abfälle möglichst gering zu halten, da der für die Ablagerung zur Verfügung stehende Raum in natürlichem Boden, beispielsweise in Salzlagerstätten, nicht unbegrenzt zur Verfügung steht.The leaching behavior of the mixture body depends strongly on its porosity. The strength of the mixture body is also influenced by the porosity. The highest possible material density should therefore be aimed for. It is also important to keep the volume to be brought into deposits for depositing the contaminated waste as low as possible, since the space available for deposit is not available in natural soil, for example in salt deposits.

Aufgabe der Erfindung ist es, ein Verfahren zum Konditionieren von trockenem kontaminierten Abfall zu schaffen, das eine hohe Konzentration von Abfall im Endprodukt bei zumindest gleichem Auslaugverhalten ermöglicht. Zugleich soll die Festigkeit des abgebundenen und ausgehärteten Gemischkörpers, insbesondere dessen Druckfestigkeit, Oberflächenhärte und Abriebsfestigkeit verbessert werden.The object of the invention is to provide a method for conditioning dry contaminated waste which enables a high concentration of waste in the end product with at least the same leaching behavior. At the same time, the strength of the set and hardened mixture body, in particular its compressive strength, surface hardness and abrasion resistance, is to be improved.

Diese Aufgabe wird bei einem Verfahren der eingangs genannten Art durch die in Patentanspruch 1 angegebenen Maßnahme gelöst. Danach wird trockenem Abfall Zement in einer Menge von nicht weniger als ca. 50 Gew. % des Abfallgewichtes zugemischt, die trockene Abfallmenge zur Zementmenge verhält sich also maximal wie 2: 1 und variiert im Bereich zwischen 1 : 1 bis 2 : 1. Dem Gemisch wird zum Abbinden Wasser zugegeben, wobei die Wassermenge unter Berücksichtigung der Abbindereaktion gering überstöchiometrisch bemessen ist. Nach Zugeben des Wassers weist das Gemisch einen etwa erdfeuchten Zustand auf. Das Gemisch wird dann unter Druck verdichtet. Beim Abbinden des Zements härtet der den Abfall enthaltende Gemischkörper aus. Es läßt sich nach diesem Verfahren in vorteilhafter Weise der Anteil trockenen Abfalls im zu lagernden Gemischkörper gegenüber drucklos in Fässern einzementierten Abfalls etwa verdoppeln, ohne daß das Auslaugverhalten verschlechtert ist. Es entsteht darüber hinaus durch das Verpressen des nur erdfeuchten, also einen nur geringen Wasserüberschuß aufweisenden Zement/Abfallgemisches ein Endprodukt hoher Festigkeit mit geringem Oberflächenabrieb.This object is achieved in a method of the type mentioned by the measure specified in claim 1. Then dry waste cement is mixed in an amount of not less than approx. 50% by weight of the waste weight, the dry waste quantity to the cement quantity thus behaves as a maximum of 2: 1 and varies in the range between 1: 1 to 2: 1. The mixture water is added for setting, the amount of water taking into account the setting reaction is dimensioned slightly above stoichiometric. After adding the water, the mixture has an approximately earth-moist state. The mixture is then compressed under pressure. When the cement sets, the mixture body containing the waste hardens. According to this method, the proportion of dry waste in the mixture body to be stored can be approximately doubled compared to waste cemented in barrels without pressure, without the leaching behavior being impaired. In addition, the pressing of the cement / waste mixture, which is only moist and therefore only has a slight excess of water, produces an end product of high strength with little surface abrasion.

Ein Vorteil des Abbindens des Abfall/Zement-Gemisches unter Druck besteht auch darin, daß unter diesen Bedingungen eine Vorsortierung des Abfalls in Abfallasche, -schlacke, -schrott entfallen kann. Unter Druck füllen die fließfähigen Anteile des Abfall/Zement-Gemisches auch enge Hohlräume aus. Das verpreßte Gemisch weist ein geringes Volumen auf.An advantage of the setting of the waste / cement mixture under pressure is also that under these conditions a pre-sorting of the waste into waste ash, slag, and scrap can be omitted. The flowable portions of the waste / cement mixture also fill tight cavities under pressure. The compressed mixture has a small volume.

Dem Abfall/Zement-Gemisch wird nach Patentanspruch 2 Wasser bevorzugt in einem Verhältnis Wasser : Zement im Bereich von 0,29 bis 0,35 : 1 zugemischt. Dabei ist für die untere Grenze das zum Abbinden des Zements erforderliche stöchiometrische Wasser/Zement-Verhältnis maßgebend. Die obere Grenze wird durch die Verdichtbarkeit des Gemisches bestimmt, denn mit zunehmendem Wassergehalt nimmt die Porigkeit des abgebundenen Gemischkörpers zu. Der Wassergehalt ist so zu bemessen, daß unter Druck kein freies Wasser aus dem Gemisch ausgepreßt wird. Als optimal für das Verhältnis Wasser : Zement auch bei hohen Drücken hat sich ein Verhältnis von 0,3 : 1 herausgestellt, Patentanspruch 3.According to claim 2, the waste / cement mixture is preferably mixed with water in a water: cement ratio in the range from 0.29 to 0.35: 1. The stoichiometric water / cement ratio required to set the cement is decisive for the lower limit. The upper limit is determined by the compressibility of the mixture, because with increasing water content the porosity of the set mixture increases. The water content should be such that no free water is squeezed out of the mixture under pressure. A ratio of 0.3: 1 has been found to be optimal for the water: cement ratio, even at high pressures, claim 3.

Für eine ausreichende Verdichtung des Abfall/Zement-Gemisches ist zumindest ein Druck von ca. 5 MPa entsprechend 51 kp/cm2 erforderlich. Mit höherem Druck nimmt die Verdichtung des Abfall/ Zement-Gemisches unterproportional zu : bei einer Verdichtung mit einem um 8,5fach höheren Druck etwa um das 1,2-fache. Das verdichtete Gemisch wird drucklos abgebunden.A sufficient compression of the waste / cement mixture requires at least a pressure of approx. 5 MPa corresponding to 51 kp / cm 2 . The compaction of the waste / cement mixture increases disproportionately with higher pressure: with compaction with a pressure that is 8.5 times higher, about 1.2 times. The compressed mixture is set without pressure.

Die Erfindung wird nachfolgend anhand von Ausführungsbeispielen näher erläutert.The invention is explained in more detail below on the basis of exemplary embodiments.

Als Abfall wurde in einem Verbrennungsofen angefallene trockene radioaktive Asche in vorliegender heterogener Struktur, also unsortiert mit Portlandzement im Gewichtsverhältnis Asche : Zement von 2 : 1 vermischt. Zum Abbinden wurde diesem Gemisch Wasser im Verhältnis Wasser : Zement von 0,3 : 1 zugegeben. Der Gehalt an trockenem Abfall im abzubindenden Gemisch betrug also etwa 60 Gew.%. Bei bisher angewandtem drucklosen Verfahren betrugen die Massenverhältnisse Abfall: Zement etwa 0.65 : 1 und Wasser : Zement -- 0,4 : 1. Das Gemisch enthielt somit nur etwa 30 Gew.% trockenen Abfalls.Dry radioactive ash accumulated in a combustion furnace in the present heterogeneous structure, that is to say unsorted, was mixed with Portland cement in the ash: cement weight ratio of 2: 1 as waste. For setting, this mixture was water in a water: cement ratio of 0.3: 1 admitted. The dry waste content in the mixture to be set was therefore about 60% by weight. In the previously unpressurized process, the mass ratios of waste: cement were approximately 0.65: 1 and water: cement - 0.4: 1. The mixture thus contained only about 30% by weight of dry waste.

In einer Tabelle sind nachfolgend die durch Anwenden steigenden Druckes p in MPa [beziehungsweise kp/cm2] erzielten Dichten in g/cm3 nach Abbinden und Aushärtung des Gemischkörpers tabellarisch zusammengestellt.

Figure imgb0001
The table below shows the densities in g / cm 3 obtained by applying increasing pressure p in MPa [or kp / cm 2 ] after the mixture has set and hardened.
Figure imgb0001

Aus der Tabelle ist ersichtlich, daß mit einer Drucksteigerung um das 8,5fache eine Dichteänderung um etwa das 1,2fache erreichbar ist.From the table it can be seen that with a pressure increase of 8.5 times a density change of about 1.2 times can be achieved.

Trotz des hohen Gehaltes an trockenem Abfall im Gemischkörper waren die Korrosionserscheinungen nach 42tägigem Aufenthalt in deionisiertem Wasser nur gering und vergleichbar mit jenen von Gemischkörpern, die als Testkörper aus der gleichen Asche in drucklosem Zementierverfahren hergestellt worden waren und einen geringeren Abfallgehalt aufwiesen. Auch die Auslaugeigenschaften waren ähnlich. So wurden im Vergleich mit einem Körper aus abfallfreiem Zementstein, der durch Zugabe von Wasser zu Zement im Verhältnis von 0,28 : 1 drucklos erzeugt worden war und bei dem nach 14 Tagen 1,29% der Gesamtmasse ausgelaugt worden waren, bei einem drucklos hergestellten Gemischkörper mit einem Abfallgehalt von ca. 30 Gew.% im gleichen Zeitraum eine Auslaugrate von 1,45 % der Gesamtmasse, bei einem unter 7 MPa verpreßten Gemischkörper mit einem Abfallgehalt von ca. 60 Gew.% eine Auslaugung von 1,71 % der Gesamtmasse festgestellt.Despite the high content of dry waste in the mixture body, the signs of corrosion after 42 days in deionized water were only slight and comparable to those of mixture bodies that were produced as test bodies from the same ash in a pressureless cementing process and had a lower waste content. The leaching properties were also similar. Thus, in comparison with a body made of waste-free cement stone, which was produced without pressure by adding water to cement in the ratio of 0.28: 1 and in which 1.29% of the total mass had been leached out after 14 days, one was produced without pressure Mixture with a waste content of approx. 30% by weight in the same period has a leaching rate of 1.45% of the total mass, with a mixture body pressed under 7 MPa with a waste content of approx. 60% by weight a leaching of 1.71% of the total mass detected.

Durch Verpressen des AbfaII/Zement-Gemisches konnte im Vergleich mit drucklos hergestellten Gemischkörpern die Aschemasse, die in ein vorgegebenes Endvolumen einzubringen ist, um 82 % bei einem Druck von p = 5 MPa und um 117 % bei einem Druck von p = 30 MPa erhöht werden. Bevorzugt wird deshalb zumindest ein Druck von 7 MPa angewandt, Patentanspruch 4. Die Volumenverringerung beim Übergang von der Rohasche in den gepreßten, aus Asche, Zement und Wasser bestehenden Gemischkörper war erheblich. Bei einem Druck von p = 25 MPa ergab sich eine Volumenreduktion um den Faktor 2,7 ; beim drucklosen Verfahren liegt dieser Faktor nahe 1.By pressing the waste / cement mixture, the ash mass, which is to be introduced into a given final volume, could be increased by 82% at a pressure of p = 5 MPa and by 117% at a pressure of p = 30 MPa compared to mixture bodies produced without pressure will. A pressure of at least 7 MPa is therefore preferably used, claim 4. The reduction in volume during the transition from the raw ash into the pressed mixture consisting of ash, cement and water was considerable. At a pressure of p = 25 MPa, the volume was reduced by a factor of 2.7; in the unpressurized process, this factor is close to 1.

Claims (4)

1. Process for the conditioning of contaminated waste, which is produced in particular in the form of ash after combustion of combustible waste or as dry residue in the processing of sludge, by cementing, characterized in that a cement content of no less than about 50 % by weight of the weight of the waste is added to the dry waste, that after the mixing of the waste with the cement water is admixed to the cement in a slightly more than stoichiometric ratio for the purpose of setting and the mixture is compressed under pressure and allowed to set.
2. Process according to Claim 1, characterized in that water in admixed in the weight ratio water : cement in the range from 0.29 to 0.35 : 1.
3. Process according to Claim 2, characterized in that the weight ratio water : cement is 0.3 : 1.
4. Process according to one of the above claims, characterized in that a minimum pressure of about 7 MPa is applied for the compression.
EP84114497A 1983-12-01 1984-11-29 Process for conditioning contaminated waste by coating with cement Expired EP0156001B1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AT84114497T ATE41553T1 (en) 1983-12-01 1984-11-29 PROCESS FOR CONDITIONING CONTAMINATED WASTE BY CEMENTING.

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DE3343422 1983-12-01
DE19833343422 DE3343422A1 (en) 1983-12-01 1983-12-01 METHOD FOR CONDITIONING CONTAMINATED WASTE BY CEMENTING

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EP0156001A2 EP0156001A2 (en) 1985-10-02
EP0156001A3 EP0156001A3 (en) 1986-10-15
EP0156001B1 true EP0156001B1 (en) 1989-03-15

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DE (2) DE3343422A1 (en)

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US4257912A (en) * 1978-06-12 1981-03-24 Westinghouse Electric Corp. Concrete encapsulation for spent nuclear fuel storage
DE2856875C2 (en) * 1978-12-30 1986-01-02 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Method of filling the interstices in a subterranean cavity containing radioactive waste
DE2945006C2 (en) * 1979-11-08 1987-01-15 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Process for the production of molded bodies containing highly radioactive waste
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US4379081A (en) * 1981-03-12 1983-04-05 Westinghouse Electric Corp. Method of encapsulating waste radioactive material

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JPS60150879A (en) 1985-08-08
DE3343422A1 (en) 1985-06-20
US4652404A (en) 1987-03-24
DE3477305D1 (en) 1989-04-20
ATE41553T1 (en) 1989-04-15
EP0156001A3 (en) 1986-10-15
EP0156001A2 (en) 1985-10-02

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