Interaction of actinides with aluminosilicate colloids in statu nascendi: Part I: Generation and characterization of actinide(III)-pseudocolloids

M. A. Kim; P. J. Panak; J. I. Yun; J. I. Kim; R. Klenze; K. Köhler

doi:10.1016/S0927-7757(02)00501-0

Interaction of actinides with aluminosilicate colloids in statu nascendi: Part I: Generation and characterization of actinide(III)-pseudocolloids

M. A. Kim, P. J. Panak, J. I. Yun, J. I. Kim, R. Klenze, K. Köhler

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Abstract

A study is presented to elucidate how the trivalent actinide ions become incorporated into the formation of aluminosilicate colloids. The acidic Al solution of varying concentration from 10^-5 to 10^-3 mol l^-1, containing the Am³⁺ or Cm³⁺ ion at 4.9×10^-8 mol l^-1, is titrated with the alkaline Si solution of different concentrations from 10^-5 to 10^-3 mol l^-1 to arrive at each prefixed pH from 4 to 9. The aluminosilicate precipitate is separated by filtration at 450 nm pore size. The filtrate containing ionic and colloidal species is subsequently put into filtration at 10-kDa-pore size (ca. 1.5 nm) to separate aluminosilicate colloids from ionic species in solution. The distribution of Am or Cm in the three different phases: precipitate, colloids and ionic species is analysed by radiometric measurement and the optimal conditions are ascertained for the formation of colloid-borne Am or Cm species. The particle size of the aluminosilicate colloids observed by atomic force microscope (AFM) appears to be 5-10 nm height and 10-50 nm length for most particles, whereas the average hard sphere diameter of preponderant particles evaluated by laser-induced breakdown detection (LIBD) appears to be 10-50 nm with an approximate mass concentration of 10-50 ppb. According to these data, the colloid number density may range from 10¹¹ to 10¹⁴ particles per litre solution. XPS and EDX analyses on colloids result in an atomic ratio of Al/Si to an average value of 0.7, suggesting that it may vary from 0.5 to 1.0. The speciation of colloids by time-resolved laser fluorescence spectroscopy (TRLFS) shows the formation of two different colloid-borne Cm species as coordinated with bidentate and tridentate bindings within the aluminosilicate structure. The latter species becomes predominant at pH≥6. A desorption experiment reveals that Am incorporated into aluminosilicate colloids is not dissociable at pH 7 and 9, indicating the formation of a stable colloid-borne Am species.

Original language	English
Pages (from-to)	97-108
Number of pages	12
Journal	Colloids and Surfaces A: Physicochemical and Engineering Aspects
Volume	216
Issue number	1-3
DOIs	https://doi.org/10.1016/S0927-7757(02)00501-0
State	Published - 15 Apr 2003

Keywords

Aluminosilcate-colloids
Americium
Aquatic colloids
Curium
Speciation

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10.1016/S0927-7757(02)00501-0

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@article{c97350cf68934b85be6099ae7ccd9f09,

title = "Interaction of actinides with aluminosilicate colloids in statu nascendi: Part I: Generation and characterization of actinide(III)-pseudocolloids",

abstract = "A study is presented to elucidate how the trivalent actinide ions become incorporated into the formation of aluminosilicate colloids. The acidic Al solution of varying concentration from 10-5 to 10-3 mol l-1, containing the Am3+ or Cm3+ ion at 4.9×10-8 mol l-1, is titrated with the alkaline Si solution of different concentrations from 10-5 to 10-3 mol l-1 to arrive at each prefixed pH from 4 to 9. The aluminosilicate precipitate is separated by filtration at 450 nm pore size. The filtrate containing ionic and colloidal species is subsequently put into filtration at 10-kDa-pore size (ca. 1.5 nm) to separate aluminosilicate colloids from ionic species in solution. The distribution of Am or Cm in the three different phases: precipitate, colloids and ionic species is analysed by radiometric measurement and the optimal conditions are ascertained for the formation of colloid-borne Am or Cm species. The particle size of the aluminosilicate colloids observed by atomic force microscope (AFM) appears to be 5-10 nm height and 10-50 nm length for most particles, whereas the average hard sphere diameter of preponderant particles evaluated by laser-induced breakdown detection (LIBD) appears to be 10-50 nm with an approximate mass concentration of 10-50 ppb. According to these data, the colloid number density may range from 1011 to 1014 particles per litre solution. XPS and EDX analyses on colloids result in an atomic ratio of Al/Si to an average value of 0.7, suggesting that it may vary from 0.5 to 1.0. The speciation of colloids by time-resolved laser fluorescence spectroscopy (TRLFS) shows the formation of two different colloid-borne Cm species as coordinated with bidentate and tridentate bindings within the aluminosilicate structure. The latter species becomes predominant at pH≥6. A desorption experiment reveals that Am incorporated into aluminosilicate colloids is not dissociable at pH 7 and 9, indicating the formation of a stable colloid-borne Am species.",

keywords = "Aluminosilcate-colloids, Americium, Aquatic colloids, Curium, Speciation",

author = "Kim, {M. A.} and Panak, {P. J.} and Yun, {J. I.} and Kim, {J. I.} and R. Klenze and K. K{\"o}hler",

note = "Funding Information: This work has been financially supported by the German Federal Ministry for Economy and Technology (BMWi) (Research project no. 02E9360). Thanks are due to Drs. M. Plaschke, D. Schild, and J. R{\"o}mer for the AFM, XPS and EDX analyses, C. Bitea for LIBD measurements, Drs. V. Metz and K. Dardenne for thermodynamic calculation, and Drs. H. Geckeis and A. Bauer for valuable discussion.",

year = "2003",

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doi = "10.1016/S0927-7757(02)00501-0",

language = "English",

volume = "216",

pages = "97--108",

journal = "Colloids and Surfaces A: Physicochemical and Engineering Aspects",

issn = "0927-7757",

publisher = "Elsevier",

number = "1-3",

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Interaction of actinides with aluminosilicate colloids in statu nascendi: Part I: Generation and characterization of actinide(III)-pseudocolloids. / Kim, M. A.; Panak, P. J.; Yun, J. I. et al.
In: Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 216, No. 1-3, 15.04.2003, p. 97-108.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Interaction of actinides with aluminosilicate colloids in statu nascendi

T2 - Part I: Generation and characterization of actinide(III)-pseudocolloids

AU - Kim, M. A.

AU - Panak, P. J.

AU - Yun, J. I.

AU - Kim, J. I.

AU - Klenze, R.

AU - Köhler, K.

N1 - Funding Information: This work has been financially supported by the German Federal Ministry for Economy and Technology (BMWi) (Research project no. 02E9360). Thanks are due to Drs. M. Plaschke, D. Schild, and J. Römer for the AFM, XPS and EDX analyses, C. Bitea for LIBD measurements, Drs. V. Metz and K. Dardenne for thermodynamic calculation, and Drs. H. Geckeis and A. Bauer for valuable discussion.

PY - 2003/4/15

Y1 - 2003/4/15

N2 - A study is presented to elucidate how the trivalent actinide ions become incorporated into the formation of aluminosilicate colloids. The acidic Al solution of varying concentration from 10-5 to 10-3 mol l-1, containing the Am3+ or Cm3+ ion at 4.9×10-8 mol l-1, is titrated with the alkaline Si solution of different concentrations from 10-5 to 10-3 mol l-1 to arrive at each prefixed pH from 4 to 9. The aluminosilicate precipitate is separated by filtration at 450 nm pore size. The filtrate containing ionic and colloidal species is subsequently put into filtration at 10-kDa-pore size (ca. 1.5 nm) to separate aluminosilicate colloids from ionic species in solution. The distribution of Am or Cm in the three different phases: precipitate, colloids and ionic species is analysed by radiometric measurement and the optimal conditions are ascertained for the formation of colloid-borne Am or Cm species. The particle size of the aluminosilicate colloids observed by atomic force microscope (AFM) appears to be 5-10 nm height and 10-50 nm length for most particles, whereas the average hard sphere diameter of preponderant particles evaluated by laser-induced breakdown detection (LIBD) appears to be 10-50 nm with an approximate mass concentration of 10-50 ppb. According to these data, the colloid number density may range from 1011 to 1014 particles per litre solution. XPS and EDX analyses on colloids result in an atomic ratio of Al/Si to an average value of 0.7, suggesting that it may vary from 0.5 to 1.0. The speciation of colloids by time-resolved laser fluorescence spectroscopy (TRLFS) shows the formation of two different colloid-borne Cm species as coordinated with bidentate and tridentate bindings within the aluminosilicate structure. The latter species becomes predominant at pH≥6. A desorption experiment reveals that Am incorporated into aluminosilicate colloids is not dissociable at pH 7 and 9, indicating the formation of a stable colloid-borne Am species.

AB - A study is presented to elucidate how the trivalent actinide ions become incorporated into the formation of aluminosilicate colloids. The acidic Al solution of varying concentration from 10-5 to 10-3 mol l-1, containing the Am3+ or Cm3+ ion at 4.9×10-8 mol l-1, is titrated with the alkaline Si solution of different concentrations from 10-5 to 10-3 mol l-1 to arrive at each prefixed pH from 4 to 9. The aluminosilicate precipitate is separated by filtration at 450 nm pore size. The filtrate containing ionic and colloidal species is subsequently put into filtration at 10-kDa-pore size (ca. 1.5 nm) to separate aluminosilicate colloids from ionic species in solution. The distribution of Am or Cm in the three different phases: precipitate, colloids and ionic species is analysed by radiometric measurement and the optimal conditions are ascertained for the formation of colloid-borne Am or Cm species. The particle size of the aluminosilicate colloids observed by atomic force microscope (AFM) appears to be 5-10 nm height and 10-50 nm length for most particles, whereas the average hard sphere diameter of preponderant particles evaluated by laser-induced breakdown detection (LIBD) appears to be 10-50 nm with an approximate mass concentration of 10-50 ppb. According to these data, the colloid number density may range from 1011 to 1014 particles per litre solution. XPS and EDX analyses on colloids result in an atomic ratio of Al/Si to an average value of 0.7, suggesting that it may vary from 0.5 to 1.0. The speciation of colloids by time-resolved laser fluorescence spectroscopy (TRLFS) shows the formation of two different colloid-borne Cm species as coordinated with bidentate and tridentate bindings within the aluminosilicate structure. The latter species becomes predominant at pH≥6. A desorption experiment reveals that Am incorporated into aluminosilicate colloids is not dissociable at pH 7 and 9, indicating the formation of a stable colloid-borne Am species.

KW - Aluminosilcate-colloids

KW - Americium

KW - Aquatic colloids

KW - Curium

KW - Speciation

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DO - 10.1016/S0927-7757(02)00501-0

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SN - 0927-7757

VL - 216

SP - 97

EP - 108

JO - Colloids and Surfaces A: Physicochemical and Engineering Aspects

JF - Colloids and Surfaces A: Physicochemical and Engineering Aspects

IS - 1-3

ER -

Interaction of actinides with aluminosilicate colloids in statu nascendi: Part I: Generation and characterization of actinide(III)-pseudocolloids

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