Solution Structure and Hydration Forces between Mica and Hydrophilic Versus Hydrophobic Surfaces

Nakouzi, Elias; Kerisit, Sebastien N.; Legg, Benjamine A.; Yadav, Sakshi B.; Li, Dongsheng; Stack, Andrew G.; Mundy, Christopher J.; Chun, Jaehun; Schenter, Gregory K.; De Yoreo, James J.

doi:10.1021/acs.jpcc.2c09120

Title: Solution Structure and Hydration Forces between Mica and Hydrophilic Versus Hydrophobic Surfaces

Journal Article · Thu Jan 26 00:00:00 EST 2023 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.2c09120· OSTI ID:1958177

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); City Univ. of New York (CUNY), NY (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)

Solid–liquid interfaces are central to a range of interesting phenomena including colloidal aggregation, crystallization by particle attachment, catalysis, heterogeneous nucleation, water desalination, and biomolecular assembly. While three-dimensional atomic force microscopy (3D AFM) has emerged as a technique for resolving interfacial solution structure at the molecular scale, key challenges for data interpretation persist, most notably regarding the influence of the probe on the measured structure. Using the mica–water system as a case study, we investigate the effect of hydrophilic and hydrophobic probes on interfacial solution structure measured by 3D AFM. Data from hydrophilic silicon-based probes are in good agreement with molecular dynamics simulations, wherein the innermost water molecules adsorb preferentially at the surface ditrigonal cavity sites, followed by two additional ordered hydration layers. In contrast, the hydrophobic carbon-based probes detect vertical oscillatory features but do not show lateral patterning that matches the underlying mica lattice. At high ionic strength, up to six of these oscillatory features are observed extending 2 nm into the solution phase with an average spacing of 0.29 ± (0.04) nm. We also determine that the repulsive hydration force between mica and the hydrophilic probe depends on the nature and concentration of ions in solution. Specifically, solutions with stronger ion–water and ion–ion interactions produce a stronger repulsive hydration force as the probe approaches the surface. Based on these observations, we present a scheme for controlling the outcomes of particle aggregation and attachment by varying the solution conditions to tune the hydration force.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL); Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-76RL01830; AC05-00OR22725

OSTI ID:: 1958177

Alternate ID(s):: OSTI ID: 1996636

Report Number(s):: PNNL-SA-179604

Journal Information:: Journal of Physical Chemistry. C, Vol. 127, Issue 5; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
hydration layers
interfacial viscosity
solid-liquid interface
hydrophilic
hydrophobic
mica

Title: Solution Structure and Hydration Forces between Mica and Hydrophilic Versus Hydrophobic Surfaces

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