Nonclassical Behavior in Competitive Ion Adsorption at a Charged Solid–Water Interface

Lee, Sang Soo; Park, Changyong; Sturchio, Neil C.; Fenter, Paul

doi:10.1021/acs.jpclett.0c00808

Nonclassical Behavior in Competitive Ion Adsorption at a Charged Solid–Water Interface

Journal Article · Wed Apr 15 00:00:00 EDT 2020 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.0c00808· OSTI ID:1617653

^[1]; Park, Changyong ^[1]; ^[2]; ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Delaware, Newark, DE (United States)

Ion adsorption at solid-water interfaces is commonly described by interactions between specific surface sites and adsorbed ions in classical models. However, energetic contributions from non-site-specific ion-ion interactions have not been explored systematically. Here, we report non-classical behaviors observed during competitive adsorption between Sr²⁺ and Na⁺/Rb⁺ at the negatively-charged muscovite mica (001)-water interface, revealing apparent controls of adsorbed ion speciation over the interfacial reactivity. In the absence of competing cations, Sr²⁺ adsorbs in approximately equivalent proportions of inner-sphere and outer-sphere complexes, whereas it adsorbs predominantly as an outer-sphere complex in the presence of Na⁺/Rb⁺. This transformation of adsorbed Sr²⁺ speciation significantly decreases its adsorption strength, as indicated by ~15-fold shift in the Sr²⁺ adsorption edge concentration, compared to that calculated from a classical Langmuir isotherm model developed based on site-specific interactions. Finally, these observations highlight the importance of non-site-specific interactions in controlling the energetics of chemical reactions at the charged interface.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1617653

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 10 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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