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Title: A new method for in situ structural investigations of nano-sized amorphous and crystalline materials using mixed-flow reactors

Abstract

Structural investigations of amorphous and nanocrystalline phases forming in solution are historically challenging. Few methods are capable of in situ atomic structural analysis and rigorous control of the system. A mixed-flow reactor (MFR) is used for total X-ray scattering experiments to examine the short- and long-range structure of phases in situ with pair distribution function (PDF) analysis. The adaptable experimental setup enables data collection for a range of different system chemistries, initial supersaturations and residence times. The age of the sample during analysis is controlled by adjusting the flow rate. Faster rates allow for younger samples to be examined, but if flow is too fast not enough data are acquired to average out excess signal noise. Slower flow rates form older samples, but at very slow speeds particles settle and block flow, clogging the system. Proper background collection and subtraction is critical for data optimization. Altogether, this MFR method is an ideal scheme for analyzing the in situ structures of phases that form during crystal growth in solution. As a proof of concept, high-resolution total X-ray scattering data of amorphous and crystalline calcium phosphates and amorphous calcium carbonate were collected for PDF analysis.

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1575251
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Acta Crystallographica. Section A, Foundations and Advances (Online)
Additional Journal Information:
Journal Name: Acta Crystallographica. Section A, Foundations and Advances (Online); Journal Volume: 75; Journal Issue: 5; Journal ID: ISSN 2053-2733
Publisher:
International Union of Crystallography
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; in situ X-ray total scattering; crystallization; amorphous calcium phosphate; amorphous calcium carbonate; pair distribution function analysis

Citation Formats

Hoeher, Alexandria J., Mergelsberg, Sebastian, Borkiewicz, Olaf J., Dove, Patricia M., and Michel, F. Marc. A new method for in situ structural investigations of nano-sized amorphous and crystalline materials using mixed-flow reactors. United States: N. p., 2019. Web. doi:10.1107/S2053273319008623.
Hoeher, Alexandria J., Mergelsberg, Sebastian, Borkiewicz, Olaf J., Dove, Patricia M., & Michel, F. Marc. A new method for in situ structural investigations of nano-sized amorphous and crystalline materials using mixed-flow reactors. United States. doi:10.1107/S2053273319008623.
Hoeher, Alexandria J., Mergelsberg, Sebastian, Borkiewicz, Olaf J., Dove, Patricia M., and Michel, F. Marc. Fri . "A new method for in situ structural investigations of nano-sized amorphous and crystalline materials using mixed-flow reactors". United States. doi:10.1107/S2053273319008623. https://www.osti.gov/servlets/purl/1575251.
@article{osti_1575251,
title = {A new method for in situ structural investigations of nano-sized amorphous and crystalline materials using mixed-flow reactors},
author = {Hoeher, Alexandria J. and Mergelsberg, Sebastian and Borkiewicz, Olaf J. and Dove, Patricia M. and Michel, F. Marc},
abstractNote = {Structural investigations of amorphous and nanocrystalline phases forming in solution are historically challenging. Few methods are capable of in situ atomic structural analysis and rigorous control of the system. A mixed-flow reactor (MFR) is used for total X-ray scattering experiments to examine the short- and long-range structure of phases in situ with pair distribution function (PDF) analysis. The adaptable experimental setup enables data collection for a range of different system chemistries, initial supersaturations and residence times. The age of the sample during analysis is controlled by adjusting the flow rate. Faster rates allow for younger samples to be examined, but if flow is too fast not enough data are acquired to average out excess signal noise. Slower flow rates form older samples, but at very slow speeds particles settle and block flow, clogging the system. Proper background collection and subtraction is critical for data optimization. Altogether, this MFR method is an ideal scheme for analyzing the in situ structures of phases that form during crystal growth in solution. As a proof of concept, high-resolution total X-ray scattering data of amorphous and crystalline calcium phosphates and amorphous calcium carbonate were collected for PDF analysis.},
doi = {10.1107/S2053273319008623},
journal = {Acta Crystallographica. Section A, Foundations and Advances (Online)},
number = 5,
volume = 75,
place = {United States},
year = {2019},
month = {8}
}

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