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Title: Switchable Chiral Selection of Aspartic Acids by Dynamic States of Brushite

Abstract

Here, we show the chiral recognition and separation of aspartic acid (Asp) enantiomers by achiral brushite due to the asymmetries of their dynamical steps in its nonequilibrium states. Growing brushite has a higher adsorption affinity to d-Asp, while l-Asp is predominant on the dissolving brushite surface. Microstructural characterization reveals that chiral selection is mainly attributed to brushite [101] steps, which exhibit two different configurations during crystal growth and dissolution, respectively, with each preferring a distinct enantiomer due to this asymmetry. Because these transition step configurations have different stabilities, they subsequently result in asymmetric adsorption. Furthermore, by varying free energy barriers through solution thermodynamic driving force (i.e., supersaturation), the dominant nonequilibrium intermediate states can be switched and chiral selection regulated. This finding highlights that the dynamic steps can be vital for chiral selection, which may provide a potential pathway for chirality generation through the dynamic nature.

Authors:
 [1];  [2];  [1];  [3];  [4]; ORCiD logo [2]; ORCiD logo [5]
  1. Zhejiang Univ. (China). Center for Biomaterials and Biopathways
  2. Zhejiang Univ. (China). Qiushi Academy for Advanced Studies
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences
  4. Rutgers Univ., New Brunswick, NJ (United States). Dept. of Chemistry and Chemical Biology, Inst. of Marine and Coastal Sciences
  5. Zhejiang Univ. (China). Center for Biomaterials and Biopathways, Qiushi Academy for Advanced Studies
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1390026
Report Number(s):
LLNL-JRNL-548392
Journal ID: ISSN 0002-7863; TRN: US1702366
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 25; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Jiang, Wenge, Pan, Haihua, Zhang, Zhisen, Qiu, S. Roger, Kim, J. Dongun, Xu, Xurong, and Tang, Ruikang. Switchable Chiral Selection of Aspartic Acids by Dynamic States of Brushite. United States: N. p., 2017. Web. doi:10.1021/jacs.7b03116.
Jiang, Wenge, Pan, Haihua, Zhang, Zhisen, Qiu, S. Roger, Kim, J. Dongun, Xu, Xurong, & Tang, Ruikang. Switchable Chiral Selection of Aspartic Acids by Dynamic States of Brushite. United States. doi:10.1021/jacs.7b03116.
Jiang, Wenge, Pan, Haihua, Zhang, Zhisen, Qiu, S. Roger, Kim, J. Dongun, Xu, Xurong, and Tang, Ruikang. Thu . "Switchable Chiral Selection of Aspartic Acids by Dynamic States of Brushite". United States. doi:10.1021/jacs.7b03116. https://www.osti.gov/servlets/purl/1390026.
@article{osti_1390026,
title = {Switchable Chiral Selection of Aspartic Acids by Dynamic States of Brushite},
author = {Jiang, Wenge and Pan, Haihua and Zhang, Zhisen and Qiu, S. Roger and Kim, J. Dongun and Xu, Xurong and Tang, Ruikang},
abstractNote = {Here, we show the chiral recognition and separation of aspartic acid (Asp) enantiomers by achiral brushite due to the asymmetries of their dynamical steps in its nonequilibrium states. Growing brushite has a higher adsorption affinity to d-Asp, while l-Asp is predominant on the dissolving brushite surface. Microstructural characterization reveals that chiral selection is mainly attributed to brushite [101] steps, which exhibit two different configurations during crystal growth and dissolution, respectively, with each preferring a distinct enantiomer due to this asymmetry. Because these transition step configurations have different stabilities, they subsequently result in asymmetric adsorption. Furthermore, by varying free energy barriers through solution thermodynamic driving force (i.e., supersaturation), the dominant nonequilibrium intermediate states can be switched and chiral selection regulated. This finding highlights that the dynamic steps can be vital for chiral selection, which may provide a potential pathway for chirality generation through the dynamic nature.},
doi = {10.1021/jacs.7b03116},
journal = {Journal of the American Chemical Society},
number = 25,
volume = 139,
place = {United States},
year = {Thu Jun 15 00:00:00 EDT 2017},
month = {Thu Jun 15 00:00:00 EDT 2017}
}

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