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Title: Sterically controlled mechanochemistry under hydrostatic pressure

Abstract

Mechanical stimuli can modify the energy landscape of chemical reactions and enable reaction pathways, offering a synthetic strategy that complements conventional chemistry. These mechanochemical mechanisms have been studied extensively in one-dimensional polymers under tensile stress using ring-opening and reorganization, polymer unzipping and disulfide reduction as model reactions. In these systems, the pulling force stretches chemical bonds, initiating the reaction. Additionally, it has been shown that forces orthogonal to the chemical bonds can alter the rate of bond dissociation. Furthermore, these bond activation mechanisms have not been possible under isotropic, compressive stress (that is, hydrostatic pressure). Here we show that mechanochemistry through isotropic compression is possible by molecularly engineering structures that can translate macroscopic isotropic stress into molecular-level anisotropic strain.

Authors:
 [1];  [1];  [2];  [3];  [4];  [5];  [1];  [3];  [3];  [6];  [7];  [6];  [8];  [1];  [1];  [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  2. Hong Kong Univ. of Science and Technology, Hong Kong (China); HKUST Fok Ying Tung Research Institute, Guangzhou (China)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. Univ. Nacional Autonoma de Mexico, Coyoacan (Mexico)
  6. Justus-Liebig Univ., Giessen (Germany)
  7. Justus-Liebig Univ., Giessen (Germany); Igo Sikorsky Kiev Polytechnic Institute, Kiev (Ukraine)
  8. Univ. of Chicago, Chicago, IL (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1437554
Report Number(s):
SLAC-PUB-17189
Journal ID: ISSN 0028-0836; nature25765
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 554; Journal Issue: 7693; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemical bonding; Electron transfer; Mechanical properties

Citation Formats

Yan, Hao, Yang, Fan, Pan, Ding, Lin, Yu, Hohman, J. Nathan, Solis-Ibarra, Diego, Li, Fei Hua, Dahl, Jeremy E. P., Carlson, Robert M. K., Tkachenko, Boryslav A., Fokin, Andrey A., Schreiner, Peter R., Galli, Giulia, Mao, Wendy L., Shen, Zhi -Xun, and Melosh, Nicholas A. Sterically controlled mechanochemistry under hydrostatic pressure. United States: N. p., 2018. Web. doi:10.1038/nature25765.
Yan, Hao, Yang, Fan, Pan, Ding, Lin, Yu, Hohman, J. Nathan, Solis-Ibarra, Diego, Li, Fei Hua, Dahl, Jeremy E. P., Carlson, Robert M. K., Tkachenko, Boryslav A., Fokin, Andrey A., Schreiner, Peter R., Galli, Giulia, Mao, Wendy L., Shen, Zhi -Xun, & Melosh, Nicholas A. Sterically controlled mechanochemistry under hydrostatic pressure. United States. doi:10.1038/nature25765.
Yan, Hao, Yang, Fan, Pan, Ding, Lin, Yu, Hohman, J. Nathan, Solis-Ibarra, Diego, Li, Fei Hua, Dahl, Jeremy E. P., Carlson, Robert M. K., Tkachenko, Boryslav A., Fokin, Andrey A., Schreiner, Peter R., Galli, Giulia, Mao, Wendy L., Shen, Zhi -Xun, and Melosh, Nicholas A. Wed . "Sterically controlled mechanochemistry under hydrostatic pressure". United States. doi:10.1038/nature25765.
@article{osti_1437554,
title = {Sterically controlled mechanochemistry under hydrostatic pressure},
author = {Yan, Hao and Yang, Fan and Pan, Ding and Lin, Yu and Hohman, J. Nathan and Solis-Ibarra, Diego and Li, Fei Hua and Dahl, Jeremy E. P. and Carlson, Robert M. K. and Tkachenko, Boryslav A. and Fokin, Andrey A. and Schreiner, Peter R. and Galli, Giulia and Mao, Wendy L. and Shen, Zhi -Xun and Melosh, Nicholas A.},
abstractNote = {Mechanical stimuli can modify the energy landscape of chemical reactions and enable reaction pathways, offering a synthetic strategy that complements conventional chemistry. These mechanochemical mechanisms have been studied extensively in one-dimensional polymers under tensile stress using ring-opening and reorganization, polymer unzipping and disulfide reduction as model reactions. In these systems, the pulling force stretches chemical bonds, initiating the reaction. Additionally, it has been shown that forces orthogonal to the chemical bonds can alter the rate of bond dissociation. Furthermore, these bond activation mechanisms have not been possible under isotropic, compressive stress (that is, hydrostatic pressure). Here we show that mechanochemistry through isotropic compression is possible by molecularly engineering structures that can translate macroscopic isotropic stress into molecular-level anisotropic strain.},
doi = {10.1038/nature25765},
journal = {Nature (London)},
number = 7693,
volume = 554,
place = {United States},
year = {Wed Feb 21 00:00:00 EST 2018},
month = {Wed Feb 21 00:00:00 EST 2018}
}

Journal Article:
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