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Title: Effect of pH on the Formation of Gibbsite-Layer Films at the Muscovite (001)–Water Interface

Abstract

The heterogeneous nucleation and growth of aluminum (oxy)hydroxide films in aqueous environments can be controlled by the speciation of dissolved Al species and the charge and structure of underlying mineral surfaces. The structure of gibbsite films nucleated at the interface between the muscovite (001) surface and 1 mM AlCl 3 solutions was investigated here as a function of pH using in situ X-ray reflectivity. The growth of well-ordered gibbsite films was observed at pH between 3 and 4, even when the solutions were undersaturated with respect to gibbsite. The ordering of these gibbsite films likely resulted from the structural similarity (i.e., epitaxy) between the basal planes of gibbsite and muscovite. The gibbsite films formed on the muscovite surface dissolved more than two orders of magnitude faster than bulk gibbsite in pH 4 HCl solution, indicating that they can be described as a metastable phase. In contrast, no film growth was observed at pH between 9 and 12 where the solutions were supersaturated with respect to gibbsite. These results indicate that adsorption and accumulation of aqueous Al(III) species (i.e., Al 3+ and AlOH 2+ at acidic pH) is a critical step for the formation of secondary minerals on the negatively chargedmore » muscovite surface.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany). Inst. of Resource Ecology
  3. Univ. of Delaware, Newark, DE (United States). Dept. of Geological Sciences
  4. Univ. of Illinois, Chicago, IL (United States). Dept. of Earth and Environmental Sciences
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Helmholtz Association of German Research Centers (Germany)
OSTI Identifier:
1505135
Grant/Contract Number:  
AC02-06CH11357; VH-NG-94
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 11; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lee, Sang Soo, Schmidt, Moritz, Sturchio, Neil C., Nagy, Kathryn L., and Fenter, Paul. Effect of pH on the Formation of Gibbsite-Layer Films at the Muscovite (001)–Water Interface. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.8b12122.
Lee, Sang Soo, Schmidt, Moritz, Sturchio, Neil C., Nagy, Kathryn L., & Fenter, Paul. Effect of pH on the Formation of Gibbsite-Layer Films at the Muscovite (001)–Water Interface. United States. doi:10.1021/acs.jpcc.8b12122.
Lee, Sang Soo, Schmidt, Moritz, Sturchio, Neil C., Nagy, Kathryn L., and Fenter, Paul. Tue . "Effect of pH on the Formation of Gibbsite-Layer Films at the Muscovite (001)–Water Interface". United States. doi:10.1021/acs.jpcc.8b12122.
@article{osti_1505135,
title = {Effect of pH on the Formation of Gibbsite-Layer Films at the Muscovite (001)–Water Interface},
author = {Lee, Sang Soo and Schmidt, Moritz and Sturchio, Neil C. and Nagy, Kathryn L. and Fenter, Paul},
abstractNote = {The heterogeneous nucleation and growth of aluminum (oxy)hydroxide films in aqueous environments can be controlled by the speciation of dissolved Al species and the charge and structure of underlying mineral surfaces. The structure of gibbsite films nucleated at the interface between the muscovite (001) surface and 1 mM AlCl3 solutions was investigated here as a function of pH using in situ X-ray reflectivity. The growth of well-ordered gibbsite films was observed at pH between 3 and 4, even when the solutions were undersaturated with respect to gibbsite. The ordering of these gibbsite films likely resulted from the structural similarity (i.e., epitaxy) between the basal planes of gibbsite and muscovite. The gibbsite films formed on the muscovite surface dissolved more than two orders of magnitude faster than bulk gibbsite in pH 4 HCl solution, indicating that they can be described as a metastable phase. In contrast, no film growth was observed at pH between 9 and 12 where the solutions were supersaturated with respect to gibbsite. These results indicate that adsorption and accumulation of aqueous Al(III) species (i.e., Al3+ and AlOH2+ at acidic pH) is a critical step for the formation of secondary minerals on the negatively charged muscovite surface.},
doi = {10.1021/acs.jpcc.8b12122},
journal = {Journal of Physical Chemistry. C},
number = 11,
volume = 123,
place = {United States},
year = {2019},
month = {2}
}

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This content will become publicly available on February 26, 2020
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