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Title: Hydrogen reverses the clustering tendency of carbon in amorphous silicon oxycarbide

Abstract

Amorphous silicon oxycarbide (SiOC) is of great technological interest. However, its atomic-level structure is not well understood. Using density functional theory calculations, we show that the clustering tendency of C atoms in SiOC is extremely sensitive to hydrogen (H): without H, the C-C interaction is attractive, leading to enrichment of aggregated SiC 4 tetrahedral units; with hydrogen, the C-C interaction is repulsive, leading to enrichment of randomly distributed SiCO 3 tetrahedral units. Our results suggest that conflicting experimental characterizations of C distributions may be due to differing amounts of H present in the samples investigated. Our work also opens a path for tailoring the properties of SiOC by using the total H content to control the C distribution.

Authors:
 [1];  [2]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering; Univ. of Electronic Science and Technology of China, Chengdu (China). Inst. of Fundamental and Frontier Sciences
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Univ. of California, Oakland, CA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Univ. of Nebraska, Lincoln, NE (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE), Nuclear Reactor Technologies (NE-7); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; National Science Foundation (NSF)
OSTI Identifier:
1565330
Grant/Contract Number:  
AC02-05CH11231; AC05-00OR22725; NE0000533
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ding, Hepeng, and Demkowicz, Michael J. Hydrogen reverses the clustering tendency of carbon in amorphous silicon oxycarbide. United States: N. p., 2015. Web. doi:10.1038/srep13051.
Ding, Hepeng, & Demkowicz, Michael J. Hydrogen reverses the clustering tendency of carbon in amorphous silicon oxycarbide. United States. doi:10.1038/srep13051.
Ding, Hepeng, and Demkowicz, Michael J. Thu . "Hydrogen reverses the clustering tendency of carbon in amorphous silicon oxycarbide". United States. doi:10.1038/srep13051. https://www.osti.gov/servlets/purl/1565330.
@article{osti_1565330,
title = {Hydrogen reverses the clustering tendency of carbon in amorphous silicon oxycarbide},
author = {Ding, Hepeng and Demkowicz, Michael J.},
abstractNote = {Amorphous silicon oxycarbide (SiOC) is of great technological interest. However, its atomic-level structure is not well understood. Using density functional theory calculations, we show that the clustering tendency of C atoms in SiOC is extremely sensitive to hydrogen (H): without H, the C-C interaction is attractive, leading to enrichment of aggregated SiC4 tetrahedral units; with hydrogen, the C-C interaction is repulsive, leading to enrichment of randomly distributed SiCO3 tetrahedral units. Our results suggest that conflicting experimental characterizations of C distributions may be due to differing amounts of H present in the samples investigated. Our work also opens a path for tailoring the properties of SiOC by using the total H content to control the C distribution.},
doi = {10.1038/srep13051},
journal = {Scientific Reports},
number = 1,
volume = 5,
place = {United States},
year = {2015},
month = {8}
}

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Cited by: 8 works
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