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Structure and Properties of "type IV" Lanthanide Nitrate Hydrate:Urea Deep Eutectic Solvents

Hammond, Oliver S. ; Bowron, Daniel T. and Edler, Karen J. LU orcid (2019) In ACS Sustainable Chemistry and Engineering 7(5). p.4932-4940
Abstract

A series of lanthanide nitrate hydrate:urea "Type IV" deep eutectic solvents (DES; Ln = Ce, Pr, Nd) were prepared and their physical properties measured, showing very high surface tension and density, with low viscosity and glass transition temperatures. Calculated Gordon parameters were similar to water, with lower molecular volumes than "Type III" DES. The LnDES were used as reaction media for efficient combustion synthesis of lanthanide oxides. The nanostructure of the Ce(NO 3 ) 3 ·6H 2 O:urea DES was... (More)

A series of lanthanide nitrate hydrate:urea "Type IV" deep eutectic solvents (DES; Ln = Ce, Pr, Nd) were prepared and their physical properties measured, showing very high surface tension and density, with low viscosity and glass transition temperatures. Calculated Gordon parameters were similar to water, with lower molecular volumes than "Type III" DES. The LnDES were used as reaction media for efficient combustion synthesis of lanthanide oxides. The nanostructure of the Ce(NO 3 ) 3 ·6H 2 O:urea DES was measured using neutron and X-ray scattering and resolved with empirical potential structure refinement (EPSR) atomistic modeling. The models showed the existence of strongly bonded yet fluxional oligomeric [-Ce-NO 3 -] polyanions and polycations. Because of the excess of the molecular component in the mixture, an intercalating H-bonded nanostructure containing mainly water and urea was observed, which can be considered as a lubricating molecular pseudophase. This dichotomous structural observation helps to explain some of the unusual physical properties such as low viscosity and high surface tension, while also challenging the fundamental definitions of DES.

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author
; and
publishing date
type
Contribution to journal
publication status
published
keywords
Deep eutectic solvents, Ionic liquids, Lanthanides, Nanostructure, Neutron scattering, Physical properties
in
ACS Sustainable Chemistry and Engineering
volume
7
issue
5
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85061902975
ISSN
2168-0485
DOI
10.1021/acssuschemeng.8b05548
language
English
LU publication?
no
additional info
Publisher Copyright: © Copyright 2019 American Chemical Society.
id
ed2bd0b4-6b19-46d9-80ad-3e76b883561f
date added to LUP
2023-03-29 11:21:52
date last changed
2023-03-30 15:12:20
@article{ed2bd0b4-6b19-46d9-80ad-3e76b883561f,
  abstract     = {{<p>                             A series of lanthanide nitrate hydrate:urea "Type IV" deep eutectic solvents (DES; Ln = Ce, Pr, Nd) were prepared and their physical properties measured, showing very high surface tension and density, with low viscosity and glass transition temperatures. Calculated Gordon parameters were similar to water, with lower molecular volumes than "Type III" DES. The LnDES were used as reaction media for efficient combustion synthesis of lanthanide oxides. The nanostructure of the Ce(NO                             <sub>3</sub>                             )                             <sub>3</sub>                             ·6H                             <sub>2</sub>                             O:urea DES was measured using neutron and X-ray scattering and resolved with empirical potential structure refinement (EPSR) atomistic modeling. The models showed the existence of strongly bonded yet fluxional oligomeric [-Ce-NO                             <sub>3</sub>                             -] polyanions and polycations. Because of the excess of the molecular component in the mixture, an intercalating H-bonded nanostructure containing mainly water and urea was observed, which can be considered as a lubricating molecular pseudophase. This dichotomous structural observation helps to explain some of the unusual physical properties such as low viscosity and high surface tension, while also challenging the fundamental definitions of DES.</p>}},
  author       = {{Hammond, Oliver S. and Bowron, Daniel T. and Edler, Karen J.}},
  issn         = {{2168-0485}},
  keywords     = {{Deep eutectic solvents; Ionic liquids; Lanthanides; Nanostructure; Neutron scattering; Physical properties}},
  language     = {{eng}},
  month        = {{03}},
  number       = {{5}},
  pages        = {{4932--4940}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Sustainable Chemistry and Engineering}},
  title        = {{Structure and Properties of "type IV" Lanthanide Nitrate Hydrate:Urea Deep Eutectic Solvents}},
  url          = {{http://dx.doi.org/10.1021/acssuschemeng.8b05548}},
  doi          = {{10.1021/acssuschemeng.8b05548}},
  volume       = {{7}},
  year         = {{2019}},
}