A diglycolamide-functionalized TREN-based dendrimer with a ‘crab-like' grip for the complexation of actinides and lanthanides

Arunasis Bhattacharyya, Andrea Leoncini, Prasanta K. Mohapatra* (Corresponding Author), Parveen K. Verma, Avinash S. Kanekar, Ashok K. Yadav, Sambhunath Jha, Dibyendu Bhattacharyya, Richard J.M. Egberink, Jurriaan Huskens, Willem Verboom (Corresponding Author)

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

1 Citation (Scopus)

Abstract

A generation 1 dendrimer, based on tris(2-aminoethyl)amine (TREN), containing six diglycolamide (DGA) pendent arms (termed TREN-G1-DGA) was synthesized and evaluated for the extraction of actinides and fission product ions. Solvent extraction studies indicated preferential extraction of Eu3+ over Am3+ with a separation factor value of ca. 4.5 in line with the extraction behaviour of multiple DGA ligands in previous reports. The distribution values of Am3+ and Eu3+ were about 12 and 9 times higher, respectively, than those obtained in the case of TREN-DGA using the 1 × 10−3 M ligand in 5% iso-decanol/95% n-dodecane at 3 M HNO3. The 1 : 1 (M : L) extracted species suggested ‘inclusion' complex formation where more than one DGA moiety participates in the complex formation. The extracted species were devoid of any inner-sphere coordinated water molecules as confirmed by luminescence spectroscopy. The structure of the complex was also studied by DFT computations and EXAFS which suggested binding of three DGA arms around the central metal ion in the absence of any inner-sphere nitrate ions.

Original languageEnglish
Pages (from-to)15164-15172
Number of pages9
JournalDalton transactions
Volume47
Issue number42
DOIs
Publication statusPublished - 1 Jan 2018

Fingerprint

Actinoid Series Elements
Dendrimers
Lanthanoid Series Elements
Complexation
Ions
Ligands
Fission products
Solvent extraction
Discrete Fourier transforms
Nitrates
Metal ions
Luminescence
Spectroscopy
Molecules
Water

Cite this

Bhattacharyya, Arunasis ; Leoncini, Andrea ; Mohapatra, Prasanta K. ; Verma, Parveen K. ; Kanekar, Avinash S. ; Yadav, Ashok K. ; Jha, Sambhunath ; Bhattacharyya, Dibyendu ; Egberink, Richard J.M. ; Huskens, Jurriaan ; Verboom, Willem. / A diglycolamide-functionalized TREN-based dendrimer with a ‘crab-like' grip for the complexation of actinides and lanthanides. In: Dalton transactions. 2018 ; Vol. 47, No. 42. pp. 15164-15172.
@article{6ca500d69ada4644810b501c1403d18e,
title = "A diglycolamide-functionalized TREN-based dendrimer with a ‘crab-like' grip for the complexation of actinides and lanthanides",
abstract = "A generation 1 dendrimer, based on tris(2-aminoethyl)amine (TREN), containing six diglycolamide (DGA) pendent arms (termed TREN-G1-DGA) was synthesized and evaluated for the extraction of actinides and fission product ions. Solvent extraction studies indicated preferential extraction of Eu3+ over Am3+ with a separation factor value of ca. 4.5 in line with the extraction behaviour of multiple DGA ligands in previous reports. The distribution values of Am3+ and Eu3+ were about 12 and 9 times higher, respectively, than those obtained in the case of TREN-DGA using the 1 × 10−3 M ligand in 5{\%} iso-decanol/95{\%} n-dodecane at 3 M HNO3. The 1 : 1 (M : L) extracted species suggested ‘inclusion' complex formation where more than one DGA moiety participates in the complex formation. The extracted species were devoid of any inner-sphere coordinated water molecules as confirmed by luminescence spectroscopy. The structure of the complex was also studied by DFT computations and EXAFS which suggested binding of three DGA arms around the central metal ion in the absence of any inner-sphere nitrate ions.",
author = "Arunasis Bhattacharyya and Andrea Leoncini and Mohapatra, {Prasanta K.} and Verma, {Parveen K.} and Kanekar, {Avinash S.} and Yadav, {Ashok K.} and Sambhunath Jha and Dibyendu Bhattacharyya and Egberink, {Richard J.M.} and Jurriaan Huskens and Willem Verboom",
year = "2018",
month = "1",
day = "1",
doi = "10.1039/c8dt03051k",
language = "English",
volume = "47",
pages = "15164--15172",
journal = "Dalton transactions",
issn = "1477-9226",
publisher = "Royal Society of Chemistry",
number = "42",

}

Bhattacharyya, A, Leoncini, A, Mohapatra, PK, Verma, PK, Kanekar, AS, Yadav, AK, Jha, S, Bhattacharyya, D, Egberink, RJM, Huskens, J & Verboom, W 2018, 'A diglycolamide-functionalized TREN-based dendrimer with a ‘crab-like' grip for the complexation of actinides and lanthanides', Dalton transactions, vol. 47, no. 42, pp. 15164-15172. https://doi.org/10.1039/c8dt03051k

A diglycolamide-functionalized TREN-based dendrimer with a ‘crab-like' grip for the complexation of actinides and lanthanides. / Bhattacharyya, Arunasis; Leoncini, Andrea; Mohapatra, Prasanta K. (Corresponding Author); Verma, Parveen K.; Kanekar, Avinash S.; Yadav, Ashok K.; Jha, Sambhunath; Bhattacharyya, Dibyendu; Egberink, Richard J.M.; Huskens, Jurriaan; Verboom, Willem (Corresponding Author).

In: Dalton transactions, Vol. 47, No. 42, 01.01.2018, p. 15164-15172.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - A diglycolamide-functionalized TREN-based dendrimer with a ‘crab-like' grip for the complexation of actinides and lanthanides

AU - Bhattacharyya, Arunasis

AU - Leoncini, Andrea

AU - Mohapatra, Prasanta K.

AU - Verma, Parveen K.

AU - Kanekar, Avinash S.

AU - Yadav, Ashok K.

AU - Jha, Sambhunath

AU - Bhattacharyya, Dibyendu

AU - Egberink, Richard J.M.

AU - Huskens, Jurriaan

AU - Verboom, Willem

PY - 2018/1/1

Y1 - 2018/1/1

N2 - A generation 1 dendrimer, based on tris(2-aminoethyl)amine (TREN), containing six diglycolamide (DGA) pendent arms (termed TREN-G1-DGA) was synthesized and evaluated for the extraction of actinides and fission product ions. Solvent extraction studies indicated preferential extraction of Eu3+ over Am3+ with a separation factor value of ca. 4.5 in line with the extraction behaviour of multiple DGA ligands in previous reports. The distribution values of Am3+ and Eu3+ were about 12 and 9 times higher, respectively, than those obtained in the case of TREN-DGA using the 1 × 10−3 M ligand in 5% iso-decanol/95% n-dodecane at 3 M HNO3. The 1 : 1 (M : L) extracted species suggested ‘inclusion' complex formation where more than one DGA moiety participates in the complex formation. The extracted species were devoid of any inner-sphere coordinated water molecules as confirmed by luminescence spectroscopy. The structure of the complex was also studied by DFT computations and EXAFS which suggested binding of three DGA arms around the central metal ion in the absence of any inner-sphere nitrate ions.

AB - A generation 1 dendrimer, based on tris(2-aminoethyl)amine (TREN), containing six diglycolamide (DGA) pendent arms (termed TREN-G1-DGA) was synthesized and evaluated for the extraction of actinides and fission product ions. Solvent extraction studies indicated preferential extraction of Eu3+ over Am3+ with a separation factor value of ca. 4.5 in line with the extraction behaviour of multiple DGA ligands in previous reports. The distribution values of Am3+ and Eu3+ were about 12 and 9 times higher, respectively, than those obtained in the case of TREN-DGA using the 1 × 10−3 M ligand in 5% iso-decanol/95% n-dodecane at 3 M HNO3. The 1 : 1 (M : L) extracted species suggested ‘inclusion' complex formation where more than one DGA moiety participates in the complex formation. The extracted species were devoid of any inner-sphere coordinated water molecules as confirmed by luminescence spectroscopy. The structure of the complex was also studied by DFT computations and EXAFS which suggested binding of three DGA arms around the central metal ion in the absence of any inner-sphere nitrate ions.

UR - http://www.scopus.com/inward/record.url?scp=85055640212&partnerID=8YFLogxK

U2 - 10.1039/c8dt03051k

DO - 10.1039/c8dt03051k

M3 - Article

C2 - 30311928

AN - SCOPUS:85055640212

VL - 47

SP - 15164

EP - 15172

JO - Dalton transactions

JF - Dalton transactions

SN - 1477-9226

IS - 42

ER -