DE19925601A1 - Recovery of uranium- and heavy metal-compounds from radioactive ground water by bonding with pre-treated activated carbon in an underground barrier - Google Patents

Recovery of uranium- and heavy metal-compounds from radioactive ground water by bonding with pre-treated activated carbon in an underground barrier

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Publication number
DE19925601A1
DE19925601A1 DE1999125601 DE19925601A DE19925601A1 DE 19925601 A1 DE19925601 A1 DE 19925601A1 DE 1999125601 DE1999125601 DE 1999125601 DE 19925601 A DE19925601 A DE 19925601A DE 19925601 A1 DE19925601 A1 DE 19925601A1
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Germany
Prior art keywords
activated carbon
uranium
compounds
heavy metal
groundwater
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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.)
Withdrawn
Application number
DE1999125601
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German (de)
Inventor
Eckart Buetow
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Individual
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Individual
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Application filed by Individual filed Critical Individual
Priority to DE1999125601 priority Critical patent/DE19925601A1/en
Publication of DE19925601A1 publication Critical patent/DE19925601A1/en
Withdrawn legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/68—Treatment of water, waste water, or sewage by addition of specified substances, e.g. trace elements, for ameliorating potable water
    • C02F1/683—Treatment of water, waste water, or sewage by addition of specified substances, e.g. trace elements, for ameliorating potable water by addition of complex-forming compounds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
    • B09C—RECLAMATION OF CONTAMINATED SOIL
    • B09C1/00—Reclamation of contaminated soil
    • B09C1/002—Reclamation of contaminated soil involving in-situ ground water treatment
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/28—Treatment of water, waste water, or sewage by sorption
    • C02F1/283—Treatment of water, waste water, or sewage by sorption using coal, charred products, or inorganic mixtures containing them
    • 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
    • G21F9/12—Processing by absorption; by adsorption; by ion-exchange
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/006—Radioactive compounds
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/10—Inorganic compounds
    • C02F2101/20—Heavy metals or heavy metal compounds

Abstract

A process and apparatus are claimed for recovery of dissolved uranium- and heavy metal-compounds from ground water using activated carbon, the process comprising (i) pre-treating activated carbon with natural or technical complex-formers in a tanker; and (ii) passing the contaminated ground water through an underground barrier containing the pre-treated activated carbon to bond the uranium- and heavy metal-compounds. In an alterative method the activated carbon is not pre-treated but is enriched in situ with humic compounds. This alternative method involves using a barrier which has a layer of shingle or sand joined to and upstream of the activated carbon layer. The shingle or sand layer is topped by bark mulch or peat from which the humic material is fed into the layer and hence onto the activated carbon layer.

Description

In den Jahren zwischen 1945 und 1990 wurde auf einem Gebiet von 4000 Hektar zwischen Aue im Erzgebirge und Ronneburg in Ostthüringen Uranerz abgebaut. Der durch den Bergbau entstandene Uranerz Abraum umfaßt große Halden radioaktiv strahlenden Materials, das u. a. Uran und Schwermetalle enthält. Es kommt zum Eintrag dieser Stoffe in die Grundwässer unter den Halden und der angrenzenden Gebiete und somit zu einer Belastung der Umwelt. Bisher gibt es noch keine Methode, die diesen Prozeß langfristig zu unterbinden vermag. Landschaftssanierungen, bei denen ein Tagebau mit Uranerz-Abraum gefällt wird (z. B. Tagebau Lichtenberg) verbessern zwar das äußere Bild, wirken jedoch nicht den Gefahren der unkontrollierten Verbringung von Radioaktivität in die Umwelt entgegen.Between 1945 and 1990 was on an area of 4000 hectares Uranium ore mined between Aue in the Ore Mountains and Ronneburg in East Thuringia. The uranium ore mined by mining includes large heaps of radioactive material radiant material that u. a. Contains uranium and heavy metals. There is an entry of these substances in the groundwater under the heaps and the adjacent areas and thus polluting the environment. So far there is no method that does this Long-term process can prevent. Landscaping where one Open-cast mining with uranium ore overburden (e.g. Lichtenberg open-cast mine) will improve the outer image, however, do not affect the dangers of the uncontrolled transfer of Radioactivity into the environment.

Die Erfindung stellt eine finanziell tragbare Lösung des Problems dar, die langfristig den Austrag von radioaktiven Uran- und Schwermetallverbindungen mit dem Grundwasser in das weitere Umfeld (Flüsse, Seen) durch die Reinigung des Grundwassers beim Durchströmen einer Reinigungswand (auch Reaktive Wand genannt) verhindert. Eine solche Reinigungswand ist ein in Untergrund eingebrachtes, vom Grundwasser durchströmtes Bauwerk, daß mit speziellen Sorptionsmaterialien gefüllt ist, die die Schadstoffe aus dem Grundwasser herausfiltern. Die Erfindung bezieht sich auf die Sorptionsmaterialien, die speziell für die Rückhaltung von Uran und Schwermetallen ausgerichtet sind. Grundlage ist Aktivkohle, die in der Wasseraufbereitung Verwendung findet und deren Sorptionseigenschaften durch Vorbehandlung optimiert werden.The invention represents a financially viable solution to the problem that the long term Discharge of radioactive uranium and heavy metal compounds with the groundwater in the wider environment (rivers, lakes) by cleaning up the groundwater at Flow through a cleaning wall (also called reactive wall) prevented. A such a cleaning wall is an underground one, from the groundwater flowed structure that is filled with special sorption materials that the Filter out pollutants from the groundwater. The invention relates to the Sorption materials specially designed for the retention of uranium and heavy metals are aligned. The basis is activated carbon, which is used in water treatment finds and their sorption properties are optimized by pretreatment.

Erfahrungen aus der Wasseraufbereitung haben gezeigt, daß die Adsorption von Uran- und Schwermetallverbindungen durch unbehandelte Aktivkohle unzureichend ist. Der Kernansatz der vorliegenden Erfindung besteht einerseits in der Nutzung der Eigenschaft von Uran- und Schwermetallverbindungen mit organischen Stoffen komplexe Verbindungen einzugehen und andererseits in der Nutzung der Fähigkeit von Aktivkohle vordringlich organische Verbindungen zu binden.Experience from water treatment has shown that the adsorption of uranium and heavy metal compounds from untreated activated carbon is insufficient. The The core approach of the present invention is on the one hand the use of the property of uranium and heavy metal compounds with organic substances complex Make connections and on the other hand in the use of the ability of activated carbon to bind primarily organic compounds.

Das Verfahren basiert auf der Komplexierung der Uran- und Schwermetallverbindungen im radioaktiv kontaminierten Grundwasser mit natürlichen (z. B. Huminstoffen) oder technischen Komplexbildnern (z. B. EDTA, NTA) und der Reinigung des Grundwassers von diesen Komplexverbindungen durch Aktivkohle in der Reaktiven Wand. Hierbei wird zwischen zwei Methoden der Zugabe der organischen Verbindungen unterschieden:
The process is based on the complexation of uranium and heavy metal compounds in radioactively contaminated groundwater with natural (e.g. humic substances) or technical complexing agents (e.g. EDTA, NTA) and the cleaning of the groundwater from these complex compounds by activated carbon in the reactive wall . A distinction is made between two methods of adding the organic compounds:

  • 1. Vorbehandlung der Aktivkohle mit natürlichen oder technischen Komplexbildnern1. Pretreatment of the activated carbon with natural or technical complexing agents
  • 2. Kontinuierliche Zugabe von natürlichen oder technischen Komplexbildnern im Anstrom zur mit Aktivkohle gefüllten Reinigungswand.2. Continuous addition of natural or technical complexing agents in the Inflow to the cleaning wall filled with activated carbon.
Vorrichtung und Verfahren zur Schadstoffrückhaltung unter Anwendung der Methode 1)Device and method for pollutant retention using the Method 1)

Generell wird Aktivkohle zur Wasseraufbereitung in einem Tankfahrzeug angeliefert. Die Aktivkohle muß pumpfähig sein, um sie in eine Reinigungswand bzw. Adsorberwand einzubringen. Die Pumpfähigkeit bekommt Aktivkohle durch die Zugabe von Wasser. Diesem Wasser werden beim Befüllen des Tankfahrzeugs natürliche oder technische Komplexbildner zudosiert. Beim Antransport der Aktivkohle im Tankbehälter wird ein Teil der organischen Komplexe an der Aktivkohle gebunden. Somit ist die Aktivkohle beim Einpumpen in die Reaktive Wand bereits mit organischen Verbindungen angereichert. Die Uran- und Schwermetallverbindungen aus dem kontaminierten Grundwasser bilden Komplexverbindungen mit diesen organischen Verbindungen und verbleiben in der Aktivkohle.Activated carbon for water treatment is generally delivered in a tanker. The activated carbon must be pumpable in order to put it into a cleaning wall or adsorber wall bring in. The ability to pump is activated carbon by the addition of water. This water becomes natural or technical when filling the tanker Complexing agent added. When the activated carbon is transported in the tank container, a Part of the organic complexes bound to the activated carbon. So the activated carbon when pumping into the reactive wall with organic compounds enriched. The uranium and heavy metal compounds from the contaminated Groundwater forms complex compounds with these organic compounds and remain in the activated carbon.

In der Zeichnung 1 ist die Ausführung der Erfindung unter Anwendung der Methode 1) dargestellt: Die Reinigungswand befindet sich im Untergrund auf der gesamten Höhe des Grundwasserstromes und reicht bis an die Geländeoberkante. Über ein Tankfahrzeug wird die vorbehandelte Aktivkohle in die Reinigungswand gepumpt. Das kontaminierte Grundwasser strömt durch die so beladene Reinigungswand, in der der Prozeß der Reinigung des Grundwassers verläuft. 1 shows the embodiment of the invention using method 1) shown: The cleaning wall is in the underground at the entire height of the Groundwater flow and extends to the top of the site. About a tanker the pretreated activated carbon is pumped into the cleaning wall. The contaminated Groundwater flows through the cleaning wall so loaded, in which the process of Groundwater purification is ongoing.  

Vorrichtung und Verfahren zur Schadstoffrückhaltung unter Anwendung der Methode 2)Device and method for pollutant retention using the Method 2)

In der Zeichnung 2 ist die Ausführung der Erfindung unter Anwendung der Methode 2) dargestellt:
Die Reinigungswand befindet sich im Untergrund auf der gesamten Höhe des Grundwasserleiters und reicht bis an die Geländeoberkante. Über ein Tankfahrzeug wird die unbehandelte Aktivkohle in die Reinigungswand gepumpt. Dem Aktivkohlesegment in der Reaktiven Wand wird auf gesamter Höhe ein Segment, bestehend aus einem Kiesbett und einer Rindenmulch-/Torfauflage vorgeschaltet. Während die Aktivkohle nach oben hin abgedeckt wird, ist die Rindenmulch-/Torfschicht den Niederschlägen ausgesetzt, so daß auf diesem Wege Huminstoffe in das Kiesbett gelangen. Die Vorbehandlung der Aktivkohle erfolgt somit nachträglich mit dem Durchströmen des Grundwassers durch das Kiesbettfilter in Richtung der Aktivkohle. Die Uran- und Schwermetallverbindungen aus dem kontaminierten Grundwasser gehen Komplexverbindungen sowohl im Kiesbettfllter als auch in der Aktivkohle ein und verbleiben in der Aktivkohle.In the drawing 2, the implementation of the invention is shown using method 2):
The cleaning wall is located in the underground at the entire height of the aquifer and extends to the top of the site. The untreated activated carbon is pumped into the cleaning wall via a tanker. A segment consisting of a gravel bed and a bark mulch / peat layer is placed upstream of the activated carbon segment in the reactive wall. While the activated carbon is covered upwards, the bark mulch / peat layer is exposed to the precipitation, so that humic substances get into the gravel bed in this way. The pretreatment of the activated carbon is thus carried out retrospectively as the groundwater flows through the gravel bed filter in the direction of the activated carbon. The uranium and heavy metal compounds from the contaminated groundwater enter into complex compounds both in the gravel bed filter and in the activated carbon and remain in the activated carbon.

Mit dem Erschöpfen der Beladungskapazität der Aktivkohle muß bei beiden Methoden die Aktivkohle ausgetauscht und entsorgt werden. Durch ein Monitoringsystem am Auslauf der Adsorberwand läßt sich die Beladung ermitteln. Eine andere Möglichkeit besteht durch eine kontinuierliche Probenahme von Aktivkohle aus dem Reinigungselement und seiner Analytik. Zur Analytik lassen sich bestimmte Leitparameter verwenden, die einfach zu ermitteln sind.With the exhausting of the loading capacity of the activated carbon, both methods must the activated carbon can be replaced and disposed of. Through a monitoring system on The load can be determined from the outlet of the adsorber wall. Another possibility consists of the continuous sampling of activated carbon from the Cleaning element and its analytics. Certain can be used for analysis Use guiding parameters that are easy to determine.

Claims (2)

1. Vorrichtung und Verfahren zur Schadstoffrückhaltung von gelösten Uran- und Schwermetallverbindungen aus dem Grundwasser durch vorbehandelte Aktivkohle, gekennzeichnet durch folgende Merkmale:
  • a) Aktivkohle wird beim Antransport im Tankfahrzeug mit natürlichen oder technischen Komplexbildnern vorbehandelt.
  • b) Eine Reinigungswand, in die die vorbehandelte Aktivkohle eingebracht wird, steht im unterirdischen Grundwasserstrom.
  • c) Grundwasser, kontaminiert mit gelösten radioaktiven Uran- und Schwermetallverbindungen, durchströmt die Reinigungswand.
  • d) Beim Kontakt des kontaminierten Grundwassers mit der Aktivkohle in der Reinigungswand werden die Uran- und Schwermetailverbindungen an die Aktivkohle gebunden.
1. Device and method for pollutant retention of dissolved uranium and heavy metal compounds from the groundwater by pretreated activated carbon, characterized by the following features:
  • a) Activated carbon is pretreated with natural or technical complexing agents when it is transported in the tanker.
  • b) A cleaning wall, into which the pretreated activated carbon is placed, is in the underground groundwater flow.
  • c) Groundwater, contaminated with dissolved radioactive uranium and heavy metal compounds, flows through the cleaning wall.
  • d) When the contaminated groundwater comes into contact with the activated carbon in the cleaning wall, the uranium and heavy detail compounds are bound to the activated carbon.
2. Vorrichtung und Verfahren nach Anspruch 1, dadurch gekennzeichnet, daß
  • a) man im Verfahrensschritt a) die Aktivkohle unbehandelt antransportiert,
  • b) im Verfahrensschritt b) die Aktivkohle unbehandelt in die Reinigungswand, die im unterirdischen Grundwasserstrom steht, eingebracht wird,
  • c) der Reinigungswand ein Segment vorgeschaltet wird, das aus einem Kiesbett und einer Rindenmulch-/Torfauflage besteht und
  • d) aus dieser Auflage Huminstoffe in das Kiesbett und anschließend mit dem Grundwasserstrom in die Aktivkohle gelangen,
  • e) die Aktivkohle auf diese Weise während des Prozesses mit den Huminstoffen nachträglich angereichert wird und
  • f) die im Grundwasser gelösten Uran- und Schwermetallverbindungen im Kiesbett und in der Aktivkohle Komplexverbindungen eingehen und an die Aktivkohle gebunden werden.
2. Device and method according to claim 1, characterized in that
  • a) in process step a) the activated carbon is transported untreated,
  • b) in process step b) the activated carbon is introduced untreated into the cleaning wall, which is in the underground groundwater flow,
  • c) the cleaning wall is preceded by a segment consisting of a gravel bed and a bark mulch / peat layer and
  • d) from this edition, humic substances enter the gravel bed and then the activated carbon with the groundwater flow,
  • e) the activated carbon is subsequently enriched with the humic substances during the process and
  • f) the uranium and heavy metal compounds dissolved in the groundwater enter into complex compounds in the gravel bed and in the activated carbon and are bound to the activated carbon.
DE1999125601 1999-06-04 1999-06-04 Recovery of uranium- and heavy metal-compounds from radioactive ground water by bonding with pre-treated activated carbon in an underground barrier Withdrawn DE19925601A1 (en)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2005050668A1 (en) * 2003-11-21 2005-06-02 Kapitonov Oleksandr Oleksandro Device for electrochemically deactivating metallic equipment
WO2005062314A1 (en) * 2003-12-22 2005-07-07 Kapitonov Oleksandr Oleksandro Method for removing radioactive substances from liquid wastes and discharged waters
WO2011042671A1 (en) 2009-10-08 2011-04-14 Pe@Rl Method for the oxidation treatment of a substrate for the adsorption of radionuclides
EP2742996A1 (en) 2012-12-17 2014-06-18 Latvijas Universitate Sorbents and method for synthesis of sorbents intended for removal of radionuclides and toxic trace elements from water
WO2019068289A1 (en) * 2017-10-05 2019-04-11 Aquasust Gmbh & Co. Kg Method for purifying ground and surface water in the zone around exhausted open pit mines, using filter material such as biochar which is produced according to known methods of hydrolysis or htc

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DE2711587A1 (en) * 1977-03-17 1978-09-21 Kernforschungsanlage Juelich ADSORBER MATRIX WITH THE ADSORPTIVE BINDING OF SUBSTANCES PROVIDED IN SEAWATER
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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2005050668A1 (en) * 2003-11-21 2005-06-02 Kapitonov Oleksandr Oleksandro Device for electrochemically deactivating metallic equipment
WO2005062314A1 (en) * 2003-12-22 2005-07-07 Kapitonov Oleksandr Oleksandro Method for removing radioactive substances from liquid wastes and discharged waters
WO2011042671A1 (en) 2009-10-08 2011-04-14 Pe@Rl Method for the oxidation treatment of a substrate for the adsorption of radionuclides
EP2742996A1 (en) 2012-12-17 2014-06-18 Latvijas Universitate Sorbents and method for synthesis of sorbents intended for removal of radionuclides and toxic trace elements from water
WO2019068289A1 (en) * 2017-10-05 2019-04-11 Aquasust Gmbh & Co. Kg Method for purifying ground and surface water in the zone around exhausted open pit mines, using filter material such as biochar which is produced according to known methods of hydrolysis or htc

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