DE19859746A1 - Materials, for removing heavy metals and organic pollutants from contaminated water, contain cellulose or starch derivative - Google Patents
Materials, for removing heavy metals and organic pollutants from contaminated water, contain cellulose or starch derivativeInfo
- Publication number
- DE19859746A1 DE19859746A1 DE1998159746 DE19859746A DE19859746A1 DE 19859746 A1 DE19859746 A1 DE 19859746A1 DE 1998159746 DE1998159746 DE 1998159746 DE 19859746 A DE19859746 A DE 19859746A DE 19859746 A1 DE19859746 A1 DE 19859746A1
- Authority
- DE
- Germany
- Prior art keywords
- cellulose
- combination product
- product according
- starch
- products
- 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.)
- Withdrawn
Links
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
- C02F1/28—Treatment of water, waste water, or sewage by sorption
- C02F1/286—Treatment of water, waste water, or sewage by sorption using natural organic sorbents or derivatives thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/24—Naturally occurring macromolecular compounds, e.g. humic acids or their derivatives
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Analytical Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Treatment Of Water By Ion Exchange (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
Description
Die Erfindung betrifft eine Kombination aus verschiedenen Nachwachsenden Rohstoffen, die in der Lage ist, Schwermetalle und organische Schadstoffe aus kontaminierten Wässern zu entfernen. Die einzelnen Bestandteile dieses Kombinationsproduktes werden hierzu in einem bestimmten Verhältnis miteinander vermischt und in einen Formkörper überführt. Diese Kombination aus verschiedenen Naturstoffen hat gegenüber den herkömmlichen Adsorbenzien und Ionenaustauschern den Vorteil, daß Schwermetalle als auch organische Schadstoffe zur gleichen Zeit entfernt werden können.The invention relates to a combination of different renewable raw materials, which in is able to remove heavy metals and organic pollutants from contaminated waters remove. The individual components of this combination product are combined in one certain ratio mixed together and converted into a shaped body. This Combination of different natural substances compared to conventional adsorbents and ion exchangers the advantage that heavy metals as well as organic pollutants can be removed at the same time.
Die Erfindung betrifft eine Kombination Nachwachsender Rohstoffe, deren Einsatz eine Verbesserung und eine Steigerung der Effizienz zur Eliminierung von Schwermetallen und organischen Schadstoffen in der Wasserreinigungstechnik darstellt. Das äußerst preiswerte Produkt zeichnet sich außerdem durch hohe Umweltverträglichkeit und problemlose Entsorgung aus.The invention relates to a combination of renewable raw materials, the use of which Improving and increasing efficiency to eliminate heavy metals and represents organic pollutants in water purification technology. The extremely inexpensive Product is also characterized by high environmental compatibility and problem-free Disposal from.
In der Wasserreinigungstechnik besitzen die bisher eingesetzten Adsorptionsmittel wie Aktivkohle und Aktivkokse zur Entfernung organischer Schadstoffe einen großen Stellenwert. Dies gilt ebenso für die Eliminierung von Schwermetallen durch Ionenaustauscher. Doch die eingesetzten Aktivkohlen sind nicht in Lage Schwermetalle zu entfernen, ebenso können Ionenaustauscher keine organischen Schadstoffe beseitigen. Im folgenden wird das am Beispiel der Deponiesickerwasserreinigung verdeutlicht. In der Sickerwasserreinigung werden Aktivkohlen und Ionenaustauscher dann eingesetzt, wenn das Sickerwasser eine relativ geringe Schadstofffracht mit sich führt. In diesem Fall hat sich aus wirtschaftlichen Gesichtspunkten die Verfahrenskombination Filtration zur Entfernung der partikelförmigen Inhaltsstoffe, Aktivkohleadsorption zu Entfernung der organischen Schadstoffe und Ionenaustausch zur Eliminierung der Schwermetalle bewährt. In der Verfahrensführung ist allerdings festzustellen, daß die Aktivkohleadsorption und der Ionenaustausch zwei hintereinander geschaltete Prozesse sind. Außerdem werden überwiegend polymere relativ teure Ionenaustauscherharze verwendet, deren Entsorgung Probleme bereitet.In water purification technology, the adsorbents previously used have such Activated carbon and activated coke for removing organic pollutants are very important. This also applies to the elimination of heavy metals by ion exchangers. But the Activated carbons cannot remove heavy metals Ion exchangers do not remove organic pollutants. The following is an example the landfill leachate clarification. In the leachate treatment Activated carbons and ion exchangers are used when the leachate is relatively low Carries pollutant loads. In this case, the Combination of processes for the removal of particulate matter, Activated carbon adsorption for removal of organic pollutants and ion exchange Proven removal of heavy metals. However, in the conduct of the proceedings, that the activated carbon adsorption and the ion exchange are connected in series Processes are. In addition, polymeric ion exchange resins are predominantly relatively expensive used, the disposal of which causes problems.
In Patentschriften wurde keine Kombination von verschiedenen Nachwachsenden Rohstoffen zur gleichzeitigen Entfernung von Organika und Schwermetallen aus kontaminierten Wässern gefunden. In der Patentschrift DE 23 29 079 C2 wird ein Verfahren zur Modifizierung von Cellulose als Anionenaustauscher beschrieben. Zur Modifikation wird ein Epoxypropylammoniumsalz verwendet.No combination of different renewable raw materials was used in patent specifications for the simultaneous removal of organics and heavy metals from contaminated water found. Patent specification DE 23 29 079 C2 describes a method for modifying Cellulose described as an anion exchanger. For modification, a Epoxypropylammoniumsalz used.
Die Patentschrift DE 23 35 213 B2 beschreibt ein Verfahren zur Behandlung von gewerblichen Abwässern mittels Kationenaustauscher. Hierbei wird eine kationische Cellulose verwendet.The patent DE 23 35 213 B2 describes a method for the treatment of commercial Waste water using a cation exchanger. A cationic cellulose is used here.
In der Offenlegungsschrift DE 30 48 357 A1 wird ein Verfahren zur Herstellung eines Anionenaustauschers und dessen Verwendung beschrieben. Es wurde ein Cellulosederivat bei einem pH-Wert zwischen 2 und 6 mit Polyethylenimin behandelt. Der daraus gewonnene Ionenaustauscher wird einzeln oder mit aktivierter Tonerde in der Abwassertechnik eingesetzt.The published patent application DE 30 48 357 A1 describes a method for producing a Anion exchanger and its use described. A cellulose derivative was added a pH between 2 and 6 treated with polyethyleneimine. The one gained from it Ion exchanger is used individually or with activated alumina in wastewater technology.
In der Patentschrift DD 259531 A3 wird ein Verfahren zur Herstellung von niedrigsubstituierter wasserlöslicher kationischer Cellulose und Hemicellulose oder deren Derivaten beschrieben. Die Produkte werden zu diesem Zweck verethert. Substituierte Produkte können als Hilfsmittel in der Papierherstellung und Abwasserreinigung eingesetzt werden.In the patent specification DD 259531 A3 a method for the production of low substituted water soluble cationic cellulose and hemicellulose or their Derivatives described. The products are etherified for this purpose. Substituted Products can be used as aids in paper making and wastewater treatment become.
Keine der hier aufgeführten Schriften beinhaltet ein derartiges Kombinationsprodukt wie es hier zur Patentierung angemeldet wird.None of the fonts listed here contains such a combination product as it does is registered for patenting here.
Das Kombinationsprodukt hat folgende Vorteile:
The combination product has the following advantages:
- 1. Das Kombinationsprodukt ist in der Lage gleichzeitig Schwermetalle und Organika aus kontaminierten Wässern zu entfernen.1. The combination product is capable of simultaneously heavy metals and organics to remove contaminated water.
- 2. Das Kombinationsprodukt zeichnet sich gegenüber Aktivkohle und Ionenaus tauscherharzen durch einen günstigen Rohstoffpreis aus.2. The combination product is distinguished from activated carbon and ions exchange resins through a favorable raw material price.
- 3. Das Kombinationsprodukt ist in seinem Beladungsverhalten den üblichen Sorbentien ebenbürtig. 3. The combination product is the usual sorbents in its loading behavior equal.
- 4. Das Kombinationsprodukt kann in verschiedenen Mischungsverhältnissen der einzelnen Naturstoffe dem jeweiligen belasteten Wässern angepaßt werden.4. The combination product can be mixed in different proportions of each Natural substances are adapted to the respective polluted waters.
- 5. Das Kombinationsprodukt kann in verschiedenen verfahrenstechnischen Apparaten zur Wasserreinigung, wie Festbettadsorber und Rührkesseladsorber bzw. -kaskade eingesetzt werden.5. The combination product can be used in various process engineering apparatus Water purification, such as fixed bed adsorber and stirred tank adsorber or cascade become.
- 6. Das Kombinationsprodukt kann in bestehenden Anlagen zur Reinigung kontaminierter Wässer eingesetzt werden.6. The combination product can be contaminated in existing cleaning plants Waters are used.
- 7. Bei den derzeitig durchgeführten Verfahren müssen Aktivkohleadsorber und Ionenaustauschersäulen hintereinander betrieben werden. Eine Durchführung in einem Reaktor ist nicht möglich. Durch den Einsatz des Kombinationsproduktes kann die Verfahrensführung in einem Reaktor durchgeführt werden. Es ergeben sich wesentlich günstigere Anlagen und Betriebskosten.7. In the currently carried out activated carbon adsorbers and Ion exchange columns are operated in series. An implementation in one Reactor is not possible. By using the combination product, the Process control can be carried out in a reactor. There are significant cheaper facilities and operating costs.
- 8. Das Kombinationsprodukt besteht aus nachwachsenden Rohstoffen. Diese stellen quasi eine unendliche Rohstoffquelle dar. Die derzeitig verwendeten Materialien Aktivkohle und Ionenaustauscherharz bestehen aus endlichen Rohstoffquellen wie Kohle und Erdöl. Hinzu kommt, daß diese Stoffe nach ihrem "Verbrauch" ebenso wie das Kombinationsprodukt einer thermischen Entsorgung zugeführt werden. Doch die Kohle und Harze belasten bei ihrer Entsorgung die Atmosphäre zusätzlich mit CO2, während das Kombinationsprodukt quasi CO2-neutral behandelt werden kann.8. The combination product consists of renewable raw materials. These are practically an infinite source of raw materials. The materials currently used activated carbon and ion exchange resin consist of finite sources of raw materials such as coal and petroleum. In addition, these substances, like their combination product, are disposed of thermally after their "consumption". However, the coal and resins also pollute the atmosphere with CO 2 when they are disposed of, while the combination product can be treated with CO 2 neutrality.
Anhand der folgenden Beispiele und Ergebnisse soll die Brauchbarkeit der Erfindung dargestellt werden.The following examples and results are intended to illustrate the utility of the invention being represented.
Die Befunde zeigen, daß Naturstoffe prinzipiell geeignet sind, um Schwermetalle sowie chlorierte bzw. allgemeine Kohlenwasserstoffe (KW) aus Abwässern zu entfernen. Allerdings müssen sie hinsichtlich einer der Zielstellung entsprechenden Austauschkapazität modifiziert werden. So zeigt Celluloseacetat bzw. -benzoat gegenüber der extraktfreien Cellulose (EFC) bei der Adsorption von p-Chlorphenol sowie o-Nitrotoluol eine um 25% höhere Eliminierungsrate (Abb. 1). Vor allem die Celluloseacetatfaser ist zur Entfernung der untersuchten KW geeignet. Die Eliminierungsraten liegen zwischen 80 und 90%.The results show that natural substances are in principle suitable for removing heavy metals as well as chlorinated or general hydrocarbons (KW) from waste water. However, they have to be modified with regard to an exchange capacity corresponding to the objective. For example, cellulose acetate or benzoate shows a 25% higher elimination rate compared to extract-free cellulose (EFC) in the adsorption of p-chlorophenol and o-nitrotoluene ( Fig. 1). The cellulose acetate fiber in particular is suitable for removing the investigated KW. The elimination rates are between 80 and 90%.
Cellulosephosphat erweist sich gegenüber Schwermetallen als idealer Ionenaustauscher, die Entfernung der Ionen bis in den ppm-Bereich ist möglich. In Abb. 2 ist das Ionenaustauschverhalten verschiedener Cellulose- sowie Stärkeprodukte dargestellt. Pb(II) läßt sich im Vergleich zu Zn(II), Cd(II) und Cr(III) am besten mit Cellulosephosphat aus der Modellösung entfernen. Cr(III) besitzt den niedrigsten Ionenaustauschgrad. In Abb. 3 ist die Zeitabhängigkeit der erreichbaren Austauschkapazität bezogen auf die spezifische Oberfläche von Cellulosephosphat dargestellt. Schon nach wenigen Minuten wird das Ionenaustauschgleichgewicht erreicht.Cellulose phosphate proves to be an ideal ion exchanger compared to heavy metals, the removal of the ions down to the ppm range is possible. Fig. 2 shows the ion exchange behavior of various cellulose and starch products. Compared to Zn (II), Cd (II) and Cr (III), Pb (II) can best be removed from the model solution with cellulose phosphate. Cr (III) has the lowest degree of ion exchange. Fig. 3 shows the time dependence of the achievable exchange capacity based on the specific surface area of cellulose phosphate. The ion exchange equilibrium is reached after only a few minutes.
Das oben Genannte macht deutlich, daß die Zielstellung dieses Forschungsvorhabens durch ein Kombinationsprodukt aus Cellulosephosphat (für den Ionenaustausch) sowie Celluloseacetat (für die Adsorption) erreichbar ist. Um ein preiswertes Verfahren zu realisieren, können die modifizierten Naturstoffe in nur geringer Konzentration mit einem weiteren kostengünstigen Naturstoff verschnitten werden. Hierzu wurden unter anderem Holzmehl, Roggenschrot, Rindenmulch, Hanf-Schäben bzw. -Fasern oder auch Zumischungen von Stärkeprodukten verwendet. Wichtig ist hierbei das optimale Mischungsverhältnis zu finden. Abb. 4 beinhaltet als Beispiel die Ergebnisse des Ionenaustausches mit einer Mischung aus Holzmehl und Cellulosephosphat bzw. Guarmehl. The above makes it clear that the objective of this research project can be achieved by a combination product of cellulose phosphate (for the ion exchange) and cellulose acetate (for the adsorption). In order to implement an inexpensive process, the modified natural substances can be blended in a low concentration with another inexpensive natural substance. For this purpose, among other things, wood flour, rye meal, bark mulch, hemp shives or fibers or admixtures of starch products were used. It is important to find the optimal mix ratio. Fig. 4 contains an example of the results of the ion exchange with a mixture of wood flour and cellulose phosphate or guar flour.
Die Kombination von Holzmehl und 20-25% Cellulosephosphat weist sehr gute Austauscheigenschaften auf. Die Schwermetalleliminierungsraten liegen für alle vier Schwermetalle bei über 90%. Ein vergleichbares Ergebnis wird mit der Kombination von Sägemehl und Guarmehl erreicht (Abb. 5). Der Zusatz der Carboxymethylstärken Vivastar P 5000 bzw. P 0100 bringt nicht den gleichen Erfolg. Steigt der Anteil der Stärkeprodukte über 30% verschlechtert sich durch die hohe Quellfähigkeit und Gelbildung die Filtrierbarkeit stark, so daß sich ein technischer Einsatz sehr schwierig gestaltet.The combination of wood flour and 20-25% cellulose phosphate has very good exchange properties. The heavy metal elimination rates for all four heavy metals are over 90%. A comparable result is achieved with the combination of sawdust and guar flour ( Fig. 5). Adding Vivastar P 5000 or P 0100 carboxymethyl starches does not bring the same success. If the proportion of starch products rises above 30%, the filterability deteriorates greatly due to the high swellability and gel formation, so that technical use is very difficult.
Die Tabellen 1 und 2 zeigen die in Batchversuchen erreichten Restkonzentrationen der Abwasserinhaltsstoffe mit verschiedenen Ionenaustauschern bzw. Adsorptionsmitteln auf Naturstoffbasis. Hierbei sind die hohen Ausgangskonzentrationen zu beachten, die in der Realität so selten vorkommen und immer unterschritten werden. So bewegen sich die Ausgangskonzentrationen an Schwermetallen in Rauchgasabwässern bei ca. 50 mg/l und in Bergbauabwässer des Freiberger Raumes noch darunter. Die Konzentrationen organischer Schadstoffe liegen im Durchschnitt bei maximal 10 mg/l.Tables 1 and 2 show the residual concentrations of the in batch tests Waste water ingredients with different ion exchangers or adsorbents Natural substance basis. Here, the high initial concentrations that are in the Reality happens so rarely and always falls short. That's how they move Initial concentrations of heavy metals in flue gas waste water at approx. 50 mg / l and in Mining wastewater from the Freiberg area still below. The concentrations of organic On average, pollutants are a maximum of 10 mg / l.
Prinzipiell wird deutlich, daß eine Kombination von langfaserigen Naturstoffen mit modifizierten Cellulose- bzw. Stärkeprodukten zur Schadstoffeliminierung zu bevorzugen ist. In principle, it is clear that a combination of long-fiber natural products with modified cellulose or starch products is preferred for eliminating pollutants.
Claims (7)
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DE1998159746 DE19859746A1 (en) | 1998-12-23 | 1998-12-23 | Materials, for removing heavy metals and organic pollutants from contaminated water, contain cellulose or starch derivative |
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Cited By (11)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2003011453A1 (en) * | 2001-07-26 | 2003-02-13 | Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. | Adsorber materials made of renewable raw materials, method for the production thereof and their use |
EP1433753A1 (en) * | 2002-12-20 | 2004-06-30 | ATC Dr. Mann e.K. | Use of renewable raw materials for the decontamination of waters contaminated with pharmaceuticals |
FR2872063A1 (en) * | 2004-06-29 | 2005-12-30 | Rhodia Cons Spec Ltd | USE OF POSSIBLY MODIFIED AND POSSIBLY INSOLUBLE STARCH FOR THE REMOVAL OF NATURAL ORGANIC MATERIALS IN LIQUIDS |
FR2872064A1 (en) * | 2004-06-29 | 2005-12-30 | Rhodia Cons Spec Ltd | USE OF VEGETABLE GUM POSSIBLY MODIFIED AND POSSIBLY INSOLUBLE FOR THE REMOVAL OF NATURAL OR SYNTHETIC ORGANIC MATERIALS IN LIQUIDS |
EP1795541A1 (en) * | 2004-09-29 | 2007-06-13 | Kowa Company. Ltd. | Phosphoric ester of cellulose derivative and metal adsorbent comprising the same |
WO2012103582A1 (en) | 2011-02-01 | 2012-08-09 | Australian Biorefining Pty Ltd | Cellulose phosphate powder product and process for manufacture thereof, and application to removal of contaminants from aqueous solutions |
CN102934581A (en) * | 2012-11-22 | 2013-02-20 | 中国科学院亚热带农业生态研究所 | Planting method of flax in heavy-metal contaminated soil |
DE102014206698A1 (en) * | 2014-04-07 | 2015-10-08 | G.U.B. Ingenieur Ag | Process and plant for sorption material fermentation |
CN105056898A (en) * | 2015-07-28 | 2015-11-18 | 湖南大学 | Modified rice straw stalk and preparation method and application thereof |
CN105126754A (en) * | 2015-09-02 | 2015-12-09 | 上海大学 | Method for removing chromium in water through biochar through corn straw |
CN108854983A (en) * | 2018-06-08 | 2018-11-23 | 盐城工学院 | Straw biological carbon gels ball and its preparation method and application |
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Cited By (15)
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WO2003011453A1 (en) * | 2001-07-26 | 2003-02-13 | Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. | Adsorber materials made of renewable raw materials, method for the production thereof and their use |
EP1433753A1 (en) * | 2002-12-20 | 2004-06-30 | ATC Dr. Mann e.K. | Use of renewable raw materials for the decontamination of waters contaminated with pharmaceuticals |
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WO2006010850A1 (en) * | 2004-06-29 | 2006-02-02 | Rhodia Uk Limited | Use of an optionally modified and optionally insoluble vegetable gum for eliminating natural or synthetic organic substances in liquids |
EP1795541A4 (en) * | 2004-09-29 | 2011-07-06 | Kowa Co | Phosphoric ester of cellulose derivative and metal adsorbent comprising the same |
EP1795541A1 (en) * | 2004-09-29 | 2007-06-13 | Kowa Company. Ltd. | Phosphoric ester of cellulose derivative and metal adsorbent comprising the same |
WO2012103582A1 (en) | 2011-02-01 | 2012-08-09 | Australian Biorefining Pty Ltd | Cellulose phosphate powder product and process for manufacture thereof, and application to removal of contaminants from aqueous solutions |
CN102934581A (en) * | 2012-11-22 | 2013-02-20 | 中国科学院亚热带农业生态研究所 | Planting method of flax in heavy-metal contaminated soil |
CN102934581B (en) * | 2012-11-22 | 2013-09-04 | 中国科学院亚热带农业生态研究所 | Planting method of flax in heavy-metal contaminated soil |
DE102014206698A1 (en) * | 2014-04-07 | 2015-10-08 | G.U.B. Ingenieur Ag | Process and plant for sorption material fermentation |
DE102014206698B4 (en) * | 2014-04-07 | 2021-02-04 | G.U.B. Ingenieur Ag | Process for removing pollutants from water and for fermentation of sorbent material |
CN105056898A (en) * | 2015-07-28 | 2015-11-18 | 湖南大学 | Modified rice straw stalk and preparation method and application thereof |
CN105126754A (en) * | 2015-09-02 | 2015-12-09 | 上海大学 | Method for removing chromium in water through biochar through corn straw |
CN108854983A (en) * | 2018-06-08 | 2018-11-23 | 盐城工学院 | Straw biological carbon gels ball and its preparation method and application |
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