Rb+ adsorption at the quartz(101)-aqueous interface: comparison of resonant anomalous x-ray reflectivity with ab initio calculations

Bellucci, Francesco; Lee, Sang Soo; Kubicki, James D.; Bandura, Andrei V.; Zhang, Zhan; Wesolowski, David J.; Fenter, Paul

doi:10.1021/jp510139t

Rb⁺ adsorption at the quartz(101)-aqueous interface: comparison of resonant anomalous x-ray reflectivity with ab initio calculations

Journal Article · Thu Jan 29 00:00:00 EST 2015 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/jp510139t· OSTI ID:1265355

Bellucci, Francesco ^[1]; Lee, Sang Soo ^[1]; Kubicki, James D. ^[2]; Bandura, Andrei V. ^[3]; Zhang, Zhan ^[4]; Wesolowski, David J. ^[5]; Fenter, Paul ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Pennsylvania State Univ., University Park, PA (United States). Department of Geosciences
St. Petersburg State University, St. Petersburg (Russia). Department of Quantum Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

We study adsorption of Rb⁺ to the quartz(101)–aqueous interface at room temperature with specular X-ray reflectivity, resonant anomalous X-ray reflectivity, and density functional theory. The interfacial water structures observed in deionized water and 10 mM RbCl solution at pH 9.8 were similar, having a first water layer at height of 1.7 ± 0.1 Å above the quartz surface and a second layer at 4.8 ± 0.1 Å and 3.9 ± 0.8 Å for the water and RbCl solutions, respectively. The adsorbed Rb⁺ distribution is broad and consists of presumed inner-sphere (IS) and outer-sphere (OS) complexes at heights of 1.8 ± 0.1 and 6.4 ± 1.0 Å, respectively. Projector-augmented planewave density functional theory (DFT) calculations of potential configurations for neutral and negatively charged quartz(101) surfaces at pH 7 and 12, respectively, reveal a water structure in agreement with experimental results. These DFT calculations also show differences in adsorbed speciation of Rb⁺ between these two conditions. At pH 7, the lowest energy structure shows that Rb⁺ adsorbs dominantly as an IS complex, whereas at pH 12 IS and OS complexes have equivalent energies. The DFT results at pH 12 are generally consistent with the two site Rb distribution observed from the X-ray data at pH 9.8, albeit with some differences that are discussed. In conclusion, surface charge estimated on the basis of the measured total Rb⁺ coverage was -0.11 C/m², in good agreement with the range of the surface charge magnitudes reported in the literature.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1265355

Alternate ID(s):: OSTI ID: 1392369

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 9 Vol. 119; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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