Extended hierarchical solvent perturbations from curved surfaces of mesoporous silica particles in a deep eutectic solvent

Hammons, Joshua A.; Zhang, Fan; Ilavsky, Jan

doi:10.1016/j.jcis.2018.02.078

Title: Extended hierarchical solvent perturbations from curved surfaces of mesoporous silica particles in a deep eutectic solvent

Journal Article · 03 March 2018 · Journal of Colloid and Interface Science

DOI: https://doi.org/10.1016/j.jcis.2018.02.078 · OSTI ID:1466360

Hammons, Joshua A. ^[1]; Zhang, Fan ^[2]; Ilavsky, Jan ^[3]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

Here, many applications of deep eutectic solvents (DES) rely on exploitation of their unique yet complex liquid structures. Due to the ionic nature of the DES components, their diffuse structures are perturbed in the presence of a charged surface. We hypothesize that it is possible to perturb the bulk DES structure far (> 100 nm) from a curved, charged surface with mesoscopic dimensions. We performed in situ, synchrotron-based ultra-small angle X-ray scattering (USAXS) experiments to study the solvent distribution near the surface of charged mesoporous silica particles (MPS) (≈ 0.5 µm in diameter) suspended in both water and a common type of DES (1:2 choline Cl-:ethylene glycol). A careful USAXS analysis reveals that the perturbation of electron density distribution within the DES extends ≈ 1 μm beyond the particle surface, and that this perturbation can be manipulated by the addition of salt ions (AgCl). The concentration of the pore-filling fluid is greatly reduced in the DES. Notably, we extracted the real-space structures of these fluctuations from the USAXS data using a simulated annealing approach that does not require a priori knowledge about the scattering form factor, and can be generalized to a wide range of complex small-angle scattering problems.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-06CH11357; AC52-07NA27344

OSTI ID:: 1466360

Alternate ID(s):: OSTI ID: 1769113

Report Number(s):: LLNL-JRNL-735609; 140715

Journal Information:: Journal of Colloid and Interface Science, Vol. 520, Issue C; ISSN 0021-9797

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
Electrostatic stabilization
Deep eutectic solvents
Pore activity
Nanoparticle stabilization
Small angle scattering
Mesoporous silica
Drug delivery
Green technology
Meso-scale solvent fluctuations
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY