Solute-solute interactions can have a dramatic impact on the permeation of solutes through dense polymeric membranes. In particular, understanding how solute-solute interactions can affect the design of osmotically driven membrane processes (ODMPs) is critical to the successful development of these emerging water treatment and energy generation processes. In this work, we investigate the influence that solute-solute interactions have on nitrate permeation through an asymmetric cellulose acetate forward osmosis membrane. A series of experiments that included systematic modifications to the cation paired with nitrate, the identity of the draw solute, and the solution pH were conducted. These experiments reveal that in the unique operating geometry of ODMPs, where solute containing solutions are present on both sides of the membrane, nitrate fluxes are significantly higher (>15 times in some cases) than predicted by existing models for solute permeation in ODMPs. The identity of the cation paired with nitrate influences the flux of nitrate; the identity of the cation in the draw solution does not affect the flux of nitrate; however, the identity of the anion in the draw solution has the most significant impact on the flux of nitrate. These results suggest that an ion exchange mechanism, which allows nitrate to switch rapidly with anions from the draw solution, is present when cellulose acetate based membranes are used in ODMPs.
Ionic conductivity is a phenomenon of great interest, not least because of its application in advanced electrochemical devices such as batteries and fuel cells. While lithium, sodium, and oxide fast ion conductors have been the subjects of much study, the advent of hydride (H − ) ion fast conductors opens up new windows in the understanding of fast ion conduction due to the fundamental simplicity of the H − ion consisting of just two electrons and one proton. Here we probe the nature of fast ion conduction in the hydride ion conductor, barium hydride (BaH 2 ). Unusually for a fast ion conductor, this material has a structure based upon a close-packed hexagonal lattice, with important analogues such as BaF 2 and Li 2 S. We elucidate how the structure of the high temperature phase of BaH 2 results in a disordered hydride sublattice. Furthermore, using novel combined quasi-elastic neutron scattering (QENS) and electrochemical impedance spectroscopy (EIS) we show how the high energy ions interact to create a concerted migration that results in macroscopic superionic conductivity via an interstitialcy mechanism.
We provide an exhaustive characterization of structural properties and nuclear dynamics in tungstic acid (WO3·H2O). To this end, we employ neutron and X-ray diffraction (ND and XRD) combined with inelastic neutron scattering (INS) and neutron Compton scattering (NCS) experiments, and we corroborate the analysis with extensive ab initio modeling. The first step in our analysis is the elucidation of the crystal structure based on the refinement of low-temperature powder ND data, extending the knowledge gained from XRD analysis of a mineral specimen of tungstite. These results are confronted with low-temperature INS experiments and zero-temperature phonon calculations. The analysis reveals an inconsistency in the definition of the structure of confined water with respect to crystallographic data, also showing a concomitant failure of the phonon calculations due to a strongly anharmonic confining potential. Extending the computational route toward ab initio MD (AIMD) simulations allows us to probe different structural configurations and provides an improved description of the vibrational dynamics as compared to high-resolution INS experiments, nevertheless, requiring the use of effective classical temperatures. The analysis of both INS and the NCS data reveals a remarkable similarity to the nuclear dynamics earlier reported for water confined in single-wall carbon nanotubes (SWNT), which has been qualitatively described as a new phase of ice. Our analysis reveals a strong two-dimensional hydrogen-bonding network, similar to the shell model for water in SWNT. The reported NCS data show narrowing of the hydrogen momentum distribution with respect to the reference ab initio calculations, indicating a great deal of conformational freedom due to spatial delocalization of protons in the ground state of the system, a clear signature of the quantum character of the nuclei.
Ammonia is now being widely considered as a carrier for low carbon hydrogen due to its favourable physical properties and the existing infrastructure for its transport, storage and distribution. The...
The performance of the hydride ion conductor Ca2NH is negatively affected by the incorporation of secondary anion sites. BaH2 reacted with N2 at 650 °C producing barium imide which has good electronic properties up to a certain concentration.
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