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Caesium incorporation and retention in illite interlayers
Abstract Radioactive caesium (chiefly 137Cs) is a major environmental pollutant. The mobility of Cs in temperate soils is primarily controlled by sorption onto clay minerals, particularly the frayed edges of illite interlayers. This paper investigates the adsorption of Cs to illite at the molecular scale, over both the short and long term. Transmission electron microscopy (TEM) images showed that after initial absorption into the frayed edges, Cs migrated into the illite interlayer becoming incorporated within the mineral structure. Caesium initially exchanged with hydrated Ca at the frayed edges, causing them to collapse. This process was irreversible as Cs held in the collapsed interlayers was not exchangeable with Ca. Over the long term Cs did not remain at the edge of the illite crystals, but diffused into the interlayers by exchange with K. Results from extended X-ray absorption fine structure spectroscopy (EXAFS) and density functional theory modelling confirmed that Cs was incorporated into the illite interlayer and revealed its bonding environment.
Graphical abstract Display Omitted
Highlights Cs irreversibly sorbs into the illite interlayer causing it to collapse. Cs incorporates into the collapsed illite interlayer through exchange with K. Cs is held in an inner-sphere complex in the collapsed interlayer.
Caesium incorporation and retention in illite interlayers
Abstract Radioactive caesium (chiefly 137Cs) is a major environmental pollutant. The mobility of Cs in temperate soils is primarily controlled by sorption onto clay minerals, particularly the frayed edges of illite interlayers. This paper investigates the adsorption of Cs to illite at the molecular scale, over both the short and long term. Transmission electron microscopy (TEM) images showed that after initial absorption into the frayed edges, Cs migrated into the illite interlayer becoming incorporated within the mineral structure. Caesium initially exchanged with hydrated Ca at the frayed edges, causing them to collapse. This process was irreversible as Cs held in the collapsed interlayers was not exchangeable with Ca. Over the long term Cs did not remain at the edge of the illite crystals, but diffused into the interlayers by exchange with K. Results from extended X-ray absorption fine structure spectroscopy (EXAFS) and density functional theory modelling confirmed that Cs was incorporated into the illite interlayer and revealed its bonding environment.
Graphical abstract Display Omitted
Highlights Cs irreversibly sorbs into the illite interlayer causing it to collapse. Cs incorporates into the collapsed illite interlayer through exchange with K. Cs is held in an inner-sphere complex in the collapsed interlayer.
Caesium incorporation and retention in illite interlayers
Fuller, Adam J. (author) / Shaw, Samuel (author) / Ward, Michael B. (author) / Haigh, Sarah J. (author) / Mosselmans, J. Frederick W. (author) / Peacock, Caroline L. (author) / Stackhouse, Stephen (author) / Dent, Andrew J. (author) / Trivedi, Divyesh (author) / Burke, Ian T. (author)
Applied Clay Science ; 108 ; 128-134
2015-02-08
7 pages
Article (Journal)
Electronic Resource
English
Caesium incorporation and retention in illite interlayers
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