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Title: Water-Mediated Surface Diffusion Mechanism Enables the Cold Sintering Process: A Combined Computational and Experimental Study

Abstract

The cold sintering process (CSP) densifies ceramics at much lower temperatures than conventional sintering processes. Several ceramics and composite systems have been successfully densified under cold sintering. For the grain growth kinetics of zinc oxide, reduced activation energies are shown, and yet the mechanism behind this growth is unknown. In this work, we investigate these mechanisms in more detail with experiments and ReaxFF molecular dynamics simulations. We investigated the recrystallization of zinc cations under various acidic conditions and found that their adsorption to the surface can be a rate-limiting factor for cold sintering. In conclusion, our studies show that surface hydroxylation in CSP does not inhibit crystallization; in contrast, by creating a surface complex, it creates an orders of magnitude acceleration in surface diffusion, and in turn, accelerates recrystallization.

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [1]
  1. Pennsylvania State Univ., University Park, PA (United States). Materials Research Inst.
  2. Pennsylvania State Univ., University Park, PA (United States). Materials Research Inst.; Xi'an Jiaotong Univ., Xi'an (China)
Publication Date:
Research Org.:
Univ. of Utah, Salt Lake City, UT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); US Air Force Office of Scientific Research (AFOSR); USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Science Foundation (NSF)
OSTI Identifier:
1597000
Alternate Identifier(s):
OSTI ID: 1560227
Grant/Contract Number:  
[SC0019285; AR0000766; FA9550‐16‐1‐0429; DMR‐1842922]
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
[ Journal Volume: 131; Journal Issue: 36]; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Sengul, Mert Y., Guo, Jing, Randall, Clive A., and van Duin, Adri C. T. Water-Mediated Surface Diffusion Mechanism Enables the Cold Sintering Process: A Combined Computational and Experimental Study. United States: N. p., 2019. Web. doi:10.1002/ange.201904738.
Sengul, Mert Y., Guo, Jing, Randall, Clive A., & van Duin, Adri C. T. Water-Mediated Surface Diffusion Mechanism Enables the Cold Sintering Process: A Combined Computational and Experimental Study. United States. doi:10.1002/ange.201904738.
Sengul, Mert Y., Guo, Jing, Randall, Clive A., and van Duin, Adri C. T. Thu . "Water-Mediated Surface Diffusion Mechanism Enables the Cold Sintering Process: A Combined Computational and Experimental Study". United States. doi:10.1002/ange.201904738.
@article{osti_1597000,
title = {Water-Mediated Surface Diffusion Mechanism Enables the Cold Sintering Process: A Combined Computational and Experimental Study},
author = {Sengul, Mert Y. and Guo, Jing and Randall, Clive A. and van Duin, Adri C. T.},
abstractNote = {The cold sintering process (CSP) densifies ceramics at much lower temperatures than conventional sintering processes. Several ceramics and composite systems have been successfully densified under cold sintering. For the grain growth kinetics of zinc oxide, reduced activation energies are shown, and yet the mechanism behind this growth is unknown. In this work, we investigate these mechanisms in more detail with experiments and ReaxFF molecular dynamics simulations. We investigated the recrystallization of zinc cations under various acidic conditions and found that their adsorption to the surface can be a rate-limiting factor for cold sintering. In conclusion, our studies show that surface hydroxylation in CSP does not inhibit crystallization; in contrast, by creating a surface complex, it creates an orders of magnitude acceleration in surface diffusion, and in turn, accelerates recrystallization.},
doi = {10.1002/ange.201904738},
journal = {Angewandte Chemie},
number = [36],
volume = [131],
place = {United States},
year = {2019},
month = {7}
}

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