Structure of water-in-salt and water-in-bisalt electrolytes

Abstract

We report a systematic diffraction study of two “water-in-salt” electrolytes and a “water-in-bisalt” electrolyte with high-energy x-ray diffraction (HEXRD) and polarized and unpolarized neutron diffraction (ND) on both H2O and...

The evolution of anionic nanoclusters at the electrode interface in water-in-salt electrolytes

“…S10 and S11 (ESI †). Although the shape of the characteristic peaks obtained from the new force field is slightly different from that of the original force field, 66 the shifts of characteristic peaks and the cumulative density profiles of ions are qualitatively consistent with the previous results.…”

Solvation Structure of Methanol-in-Salt Electrolyte Revealed by Small-Angle X-ray Scattering and Simulations

“…This phenomenon is also discovered in other electrolyte systems, i.e. water-in-salt, ,, which is interpreted as the alternations of anion–solvent–anion structure on the nanometer scale. , As the concentration of LiTFSI increases, the peak positions of the decomposed S ( q ) from TFSI – –TFSI – , TFSI – –methanol, and methanol–methanol move from lower to higher q . The decomposition of the neutron scattering S ( q ) are shown in Figure (e–h).…”

“…where the parameters a i , b i , and c are taken from Table 6.1.1.4 of Prince et al 48 The neutron scattering lengths are constants taken from Sears et al 57…”

Non-Newtonian Dynamics in Water-in-Salt Electrolytes

“…In subsequent work, Borodin et al 2 combined molecular dynamics (MD) numerical simulations with pulsed-field gradient nuclear magnetic resonance (PFG-NMR) diffusion to establish that nanoscale heterogeneity influences the structural and dynamic properties in this class of aqueous electrolytes and that the high Li + contribution to conductivity could be attributed to high salt dissociation and fast Li + (H 2 O) 4 diffusion through the water-rich nanodomain, while the negatively charged ionic framework relaxed much slower. Detailed diffraction, 3,4 quasielastic neutron scattering (QENS), 5,6 and Fourier transform infrared spectroscopy (FTIR) 6 investigations have, despite some minor quantitative differences with the MD predictions, largely confirmed this scenario. A network consisting of free species and finite clusters derived from a thermodynamic model of reversible ionic aggregation and gelation 7,8 shows similar features.…”

“…Jaeger et al have studied the bulk viscosity of water with molecular simulations based on Green–Kubo relations for the fluctuations of the pressure tensor and discussed its relation to the shear viscosity. Such a simulation involves the pressure tensor, and to compute it, one needs to track not only the atomic positions but also the velocities and forces acting in each atom, neither available in the trajectories computed in most simulations, including those reported in refs − . It is hoped that the present work might stimulate numerical studies of the bulk viscosity in water-in-salt electrolytes, such as the system studied here.…”