Real-time observation of cation exchange kinetics and dynamics at the muscovite-water interface

Lee, Sang Soo; Fenter, Paul; Nagy, Kathryn L.; Sturchio, Neil C.

doi:10.1038/ncomms15826

Real-time observation of cation exchange kinetics and dynamics at the muscovite-water interface

Journal Article · Fri Jun 09 00:00:00 EDT 2017 · Nature Communications

DOI:https://doi.org/10.1038/ncomms15826· OSTI ID:1363898

^[1]; ^[1]; Nagy, Kathryn L. ^[2]; Sturchio, Neil C. ^[3]

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

Here, ion exchange at charged solid–liquid interfaces is central to a broad range of chemical and transport phenomena. Real-time observations of adsorption/desorption at the molecular-scale elucidate exchange reaction pathways. Here, we report temporal variation in the distribution of Rb⁺ species at the muscovite (001)–water interface during exchange with Na⁺. Time-resolved resonant anomalous X-ray reflectivity measurements reveal that Rb⁺ desorption occurs over several tens of seconds during which thermodynamically stable inner-sphere Rb⁺ slowly transforms to less stable outer-sphere Rb⁺ at 25°C. In contrast, Rb⁺ adsorption is about twice as fast, proceeding quickly from Rb⁺ in the bulk solution to the stable inner-sphere species. The Arrhenius plot of the adsorption/desorption rate constants measured from 9 to 55°C shows that the pre-exponential factor for desorption is significantly smaller than for adsorption, indicating that this reduced attempt frequency of cation detachment largely explains the slow cation exchange processes at the interface.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1363898

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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