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@ARTICLE{Wilden:860529,
author = {Wilden, Andreas and Kowalski, Piotr and Klass, Larissa and
Kraus, Benjamin and Kreft, Fabian and Modolo, Giuseppe and
Li, Yan and Rothe, Jörg and Dardenne, Kathy and Geist,
Andreas and Leoncini, Andrea and Huskens, Jurriaan and
Verboom, Willem},
title = {{U}nprecedented {I}nversion of {S}electivity and
{E}xtraordinary {D}ifference in the {C}omplexation of
{T}rivalent f-{E}lements by {D}iastereomers of a
{M}ethylated {D}iglycolamide},
journal = {Chemistry - a European journal},
volume = {25},
number = {21},
issn = {0947-6539},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2019-01265},
pages = {5507-5513},
year = {2019},
abstract = {When considering f elements, solvent extraction is
primarily used for the removal of lanthanides from ore and
their recycling, as well as for the separation of actinides
from used nuclear fuel. Understanding the complexation
mechanism of metal ions with organic extractants,
particularly the influence of their molecular structure on
complex formation is of fundamental importance. Herein, we
report an extraordinary (up to two orders of magnitude)
change in the extraction efficiency of f elements with two
diastereomers of dimethyl tetraoctyl diglycolamide
(Me2‐TODGA), which only differ in the orientation of a
single methyl group. Solvent extraction techniques, extended
X‐ray absorption fine structure (EXAFS) measurements, and
density functional theory (DFT) based ab initio calculations
were used to understand their complex structures and to
explain their complexation mechanism. We show that the huge
differences observed in extraction selectivity results from
a small change in the complexation of nitrate counter‐ions
caused by the different orientation of one methyl group in
the backbone of the extractant. The obtained results give a
significant new insight into metal–ligand complexation
mechanisms, which will promote the development of more
efficient separation techniques},
cin = {IEK-6 / JARA-HPC},
ddc = {540},
cid = {I:(DE-Juel1)IEK-6-20101013 / $I:(DE-82)080012_20140620$},
pnm = {161 - Nuclear Waste Management (POF3-161) / SACSESS -
Safety of ACtinide Separation proceSSes (323282) / GENIORS -
GEN IV Integrated Oxide fuels recycling strategies (755171)
/ Atomistic modeling of radionuclide-bearing materials for
safe management of high level nuclear waste.
$(jiek61_20181101)$ / Investigation of the new materials for
safe management of high level nuclear waste.
$(jara0038_20121101)$},
pid = {G:(DE-HGF)POF3-161 / G:(EU-Grant)323282 /
G:(EU-Grant)755171 / $G:(DE-Juel1)jiek61_20181101$ /
$G:(DE-Juel1)jara0038_20121101$},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:30720905},
UT = {WOS:000466018300019},
doi = {10.1002/chem.201806161},
url = {https://juser.fz-juelich.de/record/860529},
}