Gentle soil remediation: immobilisation of heavy metals by aluminium and montmorillonite compounds
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1 Research Collection Doctoral Thesis Gentle soil remediation: immobilisation of heavy metals by aluminium and montmorillonite compounds Author(s): Lothenbach, Barbara Publication Date: 1996 Permanent Link: Rights / License: In Copyright - Non-Commercial Use Permitted This page was generated automatically upon download from the ETH Zurich Research Collection. For more information please consult the Terms of use. ETH Library
2 Diss. ETH No Gentle Soil Remediation: Immobilisation of Heavy Metals by Aluminium and Montmorillonite Compounds A dissertation submitted to the SWISS FEDERAL INSTITUTE OF TECHNOLOGY ZURICH for the degree of DOCTOR OF NATURAL SCIENCES presented by BARBARA LOTHENBACH Dipl. Umweltnaturwiss., ETH Zurich born February 12,1965 citizen of Weggis LU accepted on the recommendation of Prof. Dr. Rainer Schulin, examiner Dr. Gerhard Furrer, co-examiner Prof. Dr. Hans Stieher, co-examiner 1996
3 Summary For arable land contaminated by heavy metals, gentle remediation techniques are required that not only reduce toxicological risks, but also restore soil fertility. addition of "binding agents" that reduce the mobility and bioavailability of heavy metals is one of the potential approaches for "gentle soil remediation". The In this labo ratory study, the montmorillonite, Al-montmorillonite, Ali3-montmorillonite, and polynuclear AI13 were examined as binding agents for their efficacy in immobilis ing heavy metals. Batch experiments were performed to determine the sorption maxima of the three montmorillonite compounds for copper, zinc, and cadmium and the ph dependence of the sorption of nickel, copper, zinc, cadmium, and lead. Further, the influence of acidification and of humic acid on the interactions be tween heavy metals and binding agents was investigated. Finally, the efficacy of the binding agents to reduce heavy metal uptake by plants was studied in pot exper iments with Al-montmorillonite, gravel sludge, and montmorillonite. Al-montmorillonite, Ali3-montmorillonite, and AI13 were found to sorb sig nificant amounts of the investigated heavy metals, in particular nickel, copper, and zinc which were bound specifically. Strong sorption of nickel, copper, zinc, and cadmium on Al-montmorillonite occurred already at ph values approximately two units below the ph range in which precipitation of the hydroxide or carbonate phases was observed. small. The effect on the dissolved concentration of lead was rather The immobilisation of these heavy metal cations by Ali3-montmorillonite was restricted to a smaller ph range than the immobilisation by Al-montmoril lonite, while heavy metal sorption by polynuclear AI13 occurred in the ph range At ph 5 and 7 Al-montmorillonite showed higher sorption capacities for cop per, zinc, and cadmium than montmorillonite or Ali3-montmorillonite. These high sorption capacities allow for a corresponding low dose of binding agents for heavy metal immobilisation in soils and thus to limit the impacts on soil structure and soil biota. The immobilisation of heavy metals by montmorillonite, Al-montmoril lonite, and Ali3-montmorillonite was enhanced in the presence of humic acids. Sorption of nickel and zinc on Al-montmorillonite and Aln-montmorillonite increased during the first thirty weeks of the batch experiments. Supported by X- ray data, the slow dissolution of aluminium from aged Al-montmorillonite and Ali3-montmorillonite indicated a rearrangement of the interlayer aluminium hy-
4 Vffl Summary droxide lattice during ageing. During acidic dissolution of these binding agents, the concentrations of dissolved zinc increased slowly in close correlation with the concentrations of dissolved aluminium. It can be assumed that the small cations nickel and zinc, and probably also copper, became partially incorporated in the re arranged aluminium hydroxide lattice. No strengthening of cadmium or lead bind ing with time could be observed. It seems that these cations were to large to be in corporated in the aluminium hydroxide lattice. The ageing of the AI13 polymer did not affect heavy metal sorption. In summary, the results of the batch experiments show that in particular Almontmorillonite, but also Ali3-montmorillonite and AI13, may be suitable binding agents for the immobilisation of polluting heavy metals in soils. In pot experiments montmorillonite, Al-montmorillonite, and gravel sludge were tested to immobilise contaminant heavy metals in a neutral soil. Increasing doses of these agents resulted in the decrease of NaN03-extractable zinc and cad mium concentrations. Al-montmorillonite and gravel sludge immobilised both zinc and cadmium more efficient than montmorillonite. All three binding agents de creased zinc uptake by red clover (Trifolium pratense). The uptake of cadmium was reduced only by gravel sludge. No nutrient deficiency in the plants was found after the application of these binding agents. Remobilisation experiments with acid showed that zinc and cadmium sorbed on Al-montmorillonite or gravel sludge were less easily released than zinc and cadmium bound to montmorillonite. Only below ph 4.5, montmorillonite immobilised more cadmium than Al-montmoril lonite. Therefore, in acidic soils the use of montmorillonite instead of Al-montmo rillonite is recommended.
5 Zusammenfassung Fur schwermetallbelastete Landwirtschaftsflachen werden sanfte Sanierungsmethoden benotigt, welche nicht nur toxikologische Risiken minimieren, sondem ebenso auch die Bodenfruchtbarkeit wiederherstellen. Eine der Moglichkeiten ist die Zugabe von Bindemitteln, welche die Mobilitat und Bioverfugbarkeit von Schwermetallen herabsetzen. In der vorliegenden Arbeit wurde in Laborexperimenten die Effizienz von Montmorillonit, Al-Montmorillonit, Aln-Montmorillonit und polynuklearem AI13 in bezug auf die Immobilisierung von Schwermetallen untersucht. Batchexperimente wurden durchgefiihrt, um die Sorptionskapazitat der Bindemittel abzuschatzen und die ph-abhangigkeit der Nickel-, Kupfer-, Zink-, Cadmium- und Bleisorption zu untersuchen. Zusatzlich wurde der Einfluss der Versauerung und der Beigabe von Huminsauren auf die Bindung der Schwermetalle an die Bindemittel untersucht. In Topfexperimenten wurde untersucht, inwieweit Montmorillonit, Al-Montmorillonit und Kiesschlamm die Schwermetallaufnahme durch Pflanzen reduzieren. Al-Montmorillonit, Ali3-Montmorillonit und AI13 sorbierten signifikante Mengen der untersuchten Schwermetalle, wobei Nickel, Kupfer und Zink spezifisch gebunden wurden. Eine starke Sorption von Nickel, Kupfer, Zink und Cad mium an Al-Montmorillonit erfolgte bei durchschnittlich zwei Einheiten tieferen ph-werten als die Ausfallungen von Hydroxid- oder Carbonatphasen. auf die gelosten Bleikonzentrationen war gering. Der Effekt Ali3-Montmorillonit band diese Schwermetalle in einem engeren ph-bereich als Al-Montmorillonit. An das polynukleare AI13 wurden alle Schwermetalle im ph-bereich 6 bis 7.5 gebunden. Al-Montmorillonit wies bei ph-werten von 5 und 7 hohere Sorptionskapazitaten fiir Kupfer, Zink und Cadmium auf als Montmorillonit oder Ali3-Montmorillonit. Solch grosse Sorptionskapazitaten erlauben es, die benotigte Menge an Bindemitteln und damit auch die Nebenwirkungen auf die Bodenstruktur und die Bodenlebewesen entsprechend gering zu halten. Die Immobilisierung der Schwer metalle durch Montmorillonit, Al-Montmorillonit und Ali3-Montmorillonit wurde in Gegenwart von Huminsauren verstarkt. In Batchexperimenten verstarkte sich die Bindung der Schwermetalle an Al- Montmorillonit und Ali3-Montmorillonit im Laufe der ersten 30 Wochen. Rontgenspektren und das langsame Herauslosen des Aluminiums aus dem gealterten Al- und Ali3-Montmorillonite weisen auf eine Umlagerung des Aluminiumhy- Die
6 X Zusammenfassung droxidgitters wahrend der Alterung hin. Bei der Auflosung der Bindemittel unter stark sauren Bedingungen wurde eine enge Korrelation des herausgelosten Zinks mit dem herausgelosten Aluminium festgestellt. Es kann angenommen werden, dass die kleinen Kationen Nickel und Zink, und wahrscheinlich auch Kupfer, wahrend des Umlagerungsprozesses in das Aluminiumhydroxidgitter eingebaut wurden. Die Bindung von Cadmium und Blei verstarkte sich nicht mit der Zeit, weshalb anzunehmen ist, dass diese Kationen aufgrund sterischer Behinderung nicht eingebaut wurden. Die Alterung des Al^Polymers hatte keinen Einfluss auf die Schwermetallsorption. Die Ergebnisse der Batchexperimente zeigen, dass insbesondere Al-Montmo rillonit, aber auch Ali3-Montmorillonit und AI13 geeignete Bindemittel fur eine Sanierung von schwermetallbelasteten Boden darstellen. In Topfversuchen wurde die immobilisierende Wirkung von Montmorillonit, Al-Montmorillonit und Kiesschlamm in einem ph-neutralen Boden untersucht. Zunehmende Mengen an Bindemitteln bewirkten eine Abnahme der NaN03-extrahierbaren Zink- und Cadmiumkonzentrationen. Al-Montmorillonit und Kies schlamm immobilisieren Zink und Cadmium effizienter als Montmorillonit. Alle Bindemittel verminderten die Zinkaufnahme von Rotklee (Trifolium pratense), aber nur Kiesschlamm reduzierte die Cadmiumaufnahme. Die Anwendung dieser Bindemittel verursachte keine Mangelerscheinungen bei den Pflanzen. Remobilisierungsexperimente mit Saure zeigten, dass an Al-Montmorillonit und Kies schlamm gebundenes Zink und Cadmium weniger leicht wieder remobilisiert wer den konnte als an Montmorillonit gebundenes. Nur bei ph-werten unter 4.5 immobilisierte Montmorillonit mehr Cadmium als Al-Montmorillonit. Deshalb wird in sauren Boden eher die Anwendung von Montmorillonit als von Al-Montmoril lonit empfohlen.
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