| Title: |
Unveiling the Structure and Dynamics of Water Confined in Colloidal Boehmite Suspensions |
| Authors: |
Lawrence M. Anovitz; Gregory Schenter; Jaehun Chun; Micah P. Prange; Hsiu-Wen Wang; Tingting Liu; Yongqiang Cheng; Luke Daemen; William Smith; Xin Zhang; Carolyn I. Pearce; Matthew G. Tucker; Alexander I. Kolesnikov; Niina Jalarvo; Eugene Mamontov; Andrew G. Stack |
| Publication Year: |
2025 |
| Collection: |
Newcastle University: Figshare |
| Subject Terms: |
Biophysics; Cell Biology; Biotechnology; Ecology; Plasma Physics; Computational Biology; Space Science; Environmental Sciences not elsewhere classified; Biological Sciences not elsewhere classified; Chemical Sciences not elsewhere classified; Physical Sciences not elsewhere classified; structural hydroxyls involved; provide critical information; single water molecules; molecular dynamics simulations; 2 |
| Description: |
Thin fluid layers confined between nanoparticles play an important role in several natural and industrial systems, including radioactive wastes stored in tanks at the U.S. Department of Energy’s Hanford site. Multimodal neutron and computational approaches have been integrated to examine the properties of one, two, and four layers of water (H 2 O or D 2 O) on nanoparticulate, hydrous, or deuterated boehmite (γ-AlOOH or γ-AlOOD). Exposure of deuterated boehmite to H 2 O at 90 °C yielded rapid H/D isotopic exchange likely driven by a Grotthus-like proton-hopping mechanism. The in-plane and out-of-plane vibrations of the structural hydroxyls involved in this exchange were observed for both the hydrated and deuterated boehmite. These observations were confirmed by molecular dynamics simulations that also showed that single water molecules on the (010) surface bond to the structure via four bonds: two from hydrogens (deuteriums) on the water to surrounding oxygens and two from the water’s oxygen to surrounding OD/OH. Bulk water-like properties began to appear once four monolayers of water had been added, but steric crowding limited water diffusion rates once two monolayers had been added. The super-Arrhenius temperature dependence observed at four monolayers indicated glass-like behavior in a well-formed hydrogen-bonding network. Such a network is not sufficiently developed, however, when the surface water coverage is less than four layers. The unique nature of these layers can provide critical information for understanding forces between particles in proximity, and resultant effects on suspension rheology. |
| Document Type: |
article in journal/newspaper |
| Language: |
unknown |
| Relation: |
https://figshare.com/articles/journal_contribution/Unveiling_the_Structure_and_Dynamics_of_Water_Confined_in_Colloidal_Boehmite_Suspensions/29713335 |
| DOI: |
10.1021/acs.langmuir.5c00966.s001 |
| Availability: |
https://doi.org/10.1021/acs.langmuir.5c00966.s001; https://figshare.com/articles/journal_contribution/Unveiling_the_Structure_and_Dynamics_of_Water_Confined_in_Colloidal_Boehmite_Suspensions/29713335 |
| Rights: |
CC BY-NC 4.0 |
| Accession Number: |
edsbas.51FFDE8E |
| Database: |
BASE |