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Title: Carbon-boron clathrates as a new class of sp 3-bonded framework materials

Abstract

Carbon-based frameworks composed of sp 3 bonding represent a class of extremely lightweight strong materials, but only diamond and a handful of other compounds exist despite numerous predictions. Thus, there remains a large gap between the number of plausible structures predicted and those synthesized. We used a chemical design principle based on boron substitution to predict and synthesize a three-dimensional carbon-boron framework in a host/guest clathrate structure. The clathrate, with composition 2Sr@B 6C 6, exhibits the cubic bipartite sodalite structure (type VII clathrate) composed of sp 3-bonded truncated octahedral C 12B 12 host cages that trap Sr 2+ guest cations. The clathrate not only maintains the robust nature of diamond-like sp 3 bonding but also offers potential for a broad range of compounds with tunable properties through substitution of guest atoms within the cages.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1];  [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [1]
  1. Carnegie Inst. for Science, Washington, DC (United States)
  2. Carnegie Inst. for Science, Washington, DC (United States); Warsaw Univ. of Technology, Warszawa (Poland)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Carnegie Inst. for Science, Argonne, IL (United States). High Pressure Collaborative Access Team (HPCAT) and Geophysical Lab.
  4. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
  5. Naval Research Lab. (NRL), Washington, DC (United States)
  6. Carnegie Inst. for Science, Washington, DC (United States); Ludwig Maximilian Univ., Munich (Germany); Univ. College London (United Kingdom)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (Efree)
Sponsoring Org.:
Defense Advanced Research Projects Agency (DARPA); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; European Research Council (ERC)
OSTI Identifier:
1599069
Grant/Contract Number:  
[AC02-06CH11357; W31P4Q1310005; SC0001057; EAR-1634415; FG02-94ER14466; ToMCaT]
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
[ Journal Volume: 6; Journal Issue: 2]; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhu, Li, Borstad, Gustav M., Liu, Hanyu, Guńka, Piotr A., Guerette, Michael, Dolyniuk, Juli-Anna, Meng, Yue, Greenberg, Eran, Prakapenka, Vitali B., Chaloux, Brian L., Epshteyn, Albert, Cohen, Ronald E., and Strobel, Timothy A. Carbon-boron clathrates as a new class of sp3-bonded framework materials. United States: N. p., 2020. Web. doi:10.1126/sciadv.aay8361.
Zhu, Li, Borstad, Gustav M., Liu, Hanyu, Guńka, Piotr A., Guerette, Michael, Dolyniuk, Juli-Anna, Meng, Yue, Greenberg, Eran, Prakapenka, Vitali B., Chaloux, Brian L., Epshteyn, Albert, Cohen, Ronald E., & Strobel, Timothy A. Carbon-boron clathrates as a new class of sp3-bonded framework materials. United States. doi:10.1126/sciadv.aay8361.
Zhu, Li, Borstad, Gustav M., Liu, Hanyu, Guńka, Piotr A., Guerette, Michael, Dolyniuk, Juli-Anna, Meng, Yue, Greenberg, Eran, Prakapenka, Vitali B., Chaloux, Brian L., Epshteyn, Albert, Cohen, Ronald E., and Strobel, Timothy A. Wed . "Carbon-boron clathrates as a new class of sp3-bonded framework materials". United States. doi:10.1126/sciadv.aay8361. https://www.osti.gov/servlets/purl/1599069.
@article{osti_1599069,
title = {Carbon-boron clathrates as a new class of sp3-bonded framework materials},
author = {Zhu, Li and Borstad, Gustav M. and Liu, Hanyu and Guńka, Piotr A. and Guerette, Michael and Dolyniuk, Juli-Anna and Meng, Yue and Greenberg, Eran and Prakapenka, Vitali B. and Chaloux, Brian L. and Epshteyn, Albert and Cohen, Ronald E. and Strobel, Timothy A.},
abstractNote = {Carbon-based frameworks composed of sp3 bonding represent a class of extremely lightweight strong materials, but only diamond and a handful of other compounds exist despite numerous predictions. Thus, there remains a large gap between the number of plausible structures predicted and those synthesized. We used a chemical design principle based on boron substitution to predict and synthesize a three-dimensional carbon-boron framework in a host/guest clathrate structure. The clathrate, with composition 2Sr@B6C6, exhibits the cubic bipartite sodalite structure (type VII clathrate) composed of sp3-bonded truncated octahedral C12B12 host cages that trap Sr2+ guest cations. The clathrate not only maintains the robust nature of diamond-like sp3 bonding but also offers potential for a broad range of compounds with tunable properties through substitution of guest atoms within the cages.},
doi = {10.1126/sciadv.aay8361},
journal = {Science Advances},
number = [2],
volume = [6],
place = {United States},
year = {2020},
month = {1}
}

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