Monovalent ion adsorption at the muscovite (001)-solution interface: relationships among ion coverage and speciation, interfacial water structure, and substrate relaxation

Langmuir : the ACS Journal of Surfaces and Colloids
Sang Soo LeeNeil C Sturchio

Abstract

The interfacial structure between the muscovite (001) surface and aqueous solutions containing monovalent cations (3 × 10(-3) m Li(+), Na(+), H(3)O(+), K(+), Rb(+), or Cs(+), or 3 × 10(-2) m Li(+) or Na(+)) was measured using in situ specular X-ray reflectivity. The element-specific distribution of Rb(+) was also obtained with resonant anomalous X-ray reflectivity. The results demonstrate complex interdependencies among adsorbed cation coverage and speciation, interfacial hydration structure, and muscovite surface relaxation. Electron-density profiles of the solution near the surface varied systematically and distinctly with each adsorbed cation. Observations include a broad profile for H(3)O(+), a more structured profile for Li(+) and Na(+), and increasing electron density near the surface because of the inner-sphere adsorption of K(+), Rb(+), and Cs(+) at 1.91 ± 0.12, 1.97 ± 0.01, and 2.26 ± 0.01 Å, respectively. Estimated inner-sphere coverages increased from ~0.6 to 0.78 ± 0.01 to ~0.9 per unit cell area with decreasing cation hydration strength for K(+), Rb(+), and Cs(+), respectively. Between 7 and 12% of the Rb(+) coverage occurred as an outer-sphere species. Systematic trends in the vertical displacement of the muscovit...Continue Reading

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