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Title: Exploring dynamic surface processes during silicate mineral (wollastonite) dissolution with liquid cell

Abstract

Most liquid cell transmission electron microscopy (LC TEM) studies focus on nanoparticles or nanowires, in large part because the preparation and study of materials in this size range is straightforward. By contrast, this is not true for samples in the micrometre size range, in large part because of the difficulties associated with sample preparation starting from a ‘bulk’ material. There are also many advantages inherent to the study of micrometre-sized samples compared to their nanometre-sized counterparts. Here, we present a liquid cell transmission electron study that employed an innovative sample preparation technique using focused ion beam (FIB) milling to fabricate micrometre-sized electron transparent lamellae that were then welded to the liquid cell substrate. This technique, for which we have described in detail all of the fabrication steps, allows for samples having dimensions of several square micrometres to be observed by TEM in situ in a liquid. We applied this technique to test whether we could observe and measure in situ dissolution of a crystalline material called wollastonite, a calcium silicate mineral. More specifically, this study was used to observe and record surface dynamics associated with step and terrace edge movement, which are ultimately linked to the overall rate of dissolution.more » The wollastonite lamella underwent chemical reactions in pure deionized water at ambient temperature in a liquid cell with a 5-math formulam-spacer thickness. The movement of surface steps and terraces was measured periodically over a period of almost 5 h. Quite unexpectedly, the one-dimensional rates of retreat of these surface features were not constant, but changed over time. In addition, there were noticeable quantitative differences in retreat rates as a function crystallographic orientation, indicating that surface retreat is anisotropic. Several bulk rates of dissolution were also determined (1.6–4.2 • 10 -7 mol m -2 s -1) using the rates of retreat of representative terraces and steps, and were found to be within one order of magnitude of dissolution rates in the literature based on aqueous chemistry data.« less

Authors:
 [1];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Univ. of Grenoble Alpes, Grenoble (France). Inst. for Earth Sciences (ISTerre)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1364281
DOE Contract Number:  
AC05-00OR22725; CNMS2015-012; CNMS2014-R69; 06736
Resource Type:
Journal Article
Journal Name:
Journal of Microscopy
Additional Journal Information:
Journal Volume: 265; Journal Issue: 3; Journal ID: ISSN 0022-2720
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; Bulk dissolution rate; crystalline wollastonite mineral; lamella preparation by FIB; liquid cell TEM; step edge and terrace movement; surface retreat rates.

Citation Formats

Leonard, Donovan N., and Hellmann, Roland. Exploring dynamic surface processes during silicate mineral (wollastonite) dissolution with liquid cell. United States: N. p., 2016. Web. doi:10.1111/jmi.12509.
Leonard, Donovan N., & Hellmann, Roland. Exploring dynamic surface processes during silicate mineral (wollastonite) dissolution with liquid cell. United States. doi:10.1111/jmi.12509.
Leonard, Donovan N., and Hellmann, Roland. Mon . "Exploring dynamic surface processes during silicate mineral (wollastonite) dissolution with liquid cell". United States. doi:10.1111/jmi.12509.
@article{osti_1364281,
title = {Exploring dynamic surface processes during silicate mineral (wollastonite) dissolution with liquid cell},
author = {Leonard, Donovan N. and Hellmann, Roland},
abstractNote = {Most liquid cell transmission electron microscopy (LC TEM) studies focus on nanoparticles or nanowires, in large part because the preparation and study of materials in this size range is straightforward. By contrast, this is not true for samples in the micrometre size range, in large part because of the difficulties associated with sample preparation starting from a ‘bulk’ material. There are also many advantages inherent to the study of micrometre-sized samples compared to their nanometre-sized counterparts. Here, we present a liquid cell transmission electron study that employed an innovative sample preparation technique using focused ion beam (FIB) milling to fabricate micrometre-sized electron transparent lamellae that were then welded to the liquid cell substrate. This technique, for which we have described in detail all of the fabrication steps, allows for samples having dimensions of several square micrometres to be observed by TEM in situ in a liquid. We applied this technique to test whether we could observe and measure in situ dissolution of a crystalline material called wollastonite, a calcium silicate mineral. More specifically, this study was used to observe and record surface dynamics associated with step and terrace edge movement, which are ultimately linked to the overall rate of dissolution. The wollastonite lamella underwent chemical reactions in pure deionized water at ambient temperature in a liquid cell with a 5-math formulam-spacer thickness. The movement of surface steps and terraces was measured periodically over a period of almost 5 h. Quite unexpectedly, the one-dimensional rates of retreat of these surface features were not constant, but changed over time. In addition, there were noticeable quantitative differences in retreat rates as a function crystallographic orientation, indicating that surface retreat is anisotropic. Several bulk rates of dissolution were also determined (1.6–4.2 • 10-7 mol m-2 s-1) using the rates of retreat of representative terraces and steps, and were found to be within one order of magnitude of dissolution rates in the literature based on aqueous chemistry data.},
doi = {10.1111/jmi.12509},
journal = {Journal of Microscopy},
issn = {0022-2720},
number = 3,
volume = 265,
place = {United States},
year = {2016},
month = {12}
}

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