| Autor: |
Hammond OS; Centre for Sustainable Chemical Technologies, University of Bath, Claverton Down, Bath BA2 7AY, U.K.; Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, U.K., Bathke EK; Centre for Sustainable Chemical Technologies, University of Bath, Claverton Down, Bath BA2 7AY, U.K.; Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, U.K., Bowron DT; ISIS Neutron and Muon Source, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Didcot OX11 0QX, U.K., Edler KJ; Centre for Sustainable Chemical Technologies, University of Bath, Claverton Down, Bath BA2 7AY, U.K.; Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, U.K. |
| Abstrakt: |
Eutectic mixtures of choline chloride, urea, and water in deep eutectic solvent (DES)/water molar hydration ratios ( w ) of 2, 5, and 10, with dissolved cerium salt, were measured using neutron diffraction with isotopic substitution. Structures were modeled using empirical potential structure refinement (EPSR). Ce 3+ was found to form highly charged complexes with a mean coordination number between 7 and 8, with the shell containing mostly chloride, followed by water. The shell composition is strongly affected by the molar ratio of dilution, as opposed to the mass or volume fraction, due to the high affinity of Cl - and H 2 O ligands that displace less favorable interactions with ligands such as urea and choline. The presence of Ce 3+ salt disrupted the bulk DES structure slightly, making it more electrolyte-like. The measured coordination shell of choline showed significant discrepancies from the statistical noninteracting distribution, highlighting the nonideality of the blend. Cluster analysis revealed the trace presence of percolating water clusters (25 ≥ n ≥ 2) in solvent compositions of 5 and 10 w for the first time. |
