Route to high-energy density polymeric nitrogen t-N via He-N compounds
Abstract
Polymeric nitrogen, stabilized by compressing pure molecular nitrogen, has yet to be recovered to ambient conditions, precluding its application as a high-energy density material. Here we suggest a route for synthesis of a tetragonal polymeric nitrogen, denoted t-N, via He-N compounds at high pressures. Using first-principles calculations with structure searching, we predict a class of nitrides with stoichiometry HeN4 that are energetically stable (relative to a mixture of solid He and N2) above 8.5 GPa. At high pressure, HeN4 comprises a polymeric channel-like nitrogen framework filled with linearly arranged helium atoms. The nitrogen framework persists to ambient pressure on decompression after removal of helium, forming pure polymeric nitrogen, t-N. t-N is dynamically and mechanically stable at ambient pressure with an estimated energy density of ~11.31 kJ/g, marking it out as a remarkable high-energy density material. As a result, this expands the known polymeric forms of nitrogen and indicates a route to its synthesis.
- Authors:
-
[4];
- Jiangsu Normal Univ., Xuzhou (China)
- Jilin Univ., Changchun (China); Univ. of Cambridge, Cambridge (United Kingdom)
- Carnegie Inst. of Washington, Washington, D.C. (United States)
- Univ. of Cambridge, Cambridge (United Kingdom); Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
- Deakin Univ., Waurn Ponds, VIC (Australia)
- Jilin Univ., Changchun (China)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (EFree)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1470638
- Grant/Contract Number:
- NA0002006; SC0001057
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Related Information: EFree partners with Carnegie Institution of Washington (lead); California Institute of Technology; Colorado School of Mines; Cornell University; Lehigh University; Pennsylvania State University; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; catalysis (heterogeneous); solar (photovoltaic); phonons; thermoelectric; energy storage (including batteries and capacitors); hydrogen and fuel cells; superconductivity; charge transport; mesostructured materials; materials and chemistry by design; synthesis (novel materials)
Citation Formats
Li, Yinwei, Feng, Xiaolei, Liu, Hanyu, Hao, Jian, Redfern, Simon A. T., Lei, Weiwei, Liu, Dan, and Ma, Yanming. Route to high-energy density polymeric nitrogen t-N via He-N compounds. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-03200-4.
Li, Yinwei, Feng, Xiaolei, Liu, Hanyu, Hao, Jian, Redfern, Simon A. T., Lei, Weiwei, Liu, Dan, & Ma, Yanming. Route to high-energy density polymeric nitrogen t-N via He-N compounds. United States. https://doi.org/10.1038/s41467-018-03200-4
Li, Yinwei, Feng, Xiaolei, Liu, Hanyu, Hao, Jian, Redfern, Simon A. T., Lei, Weiwei, Liu, Dan, and Ma, Yanming. Mon .
"Route to high-energy density polymeric nitrogen t-N via He-N compounds". United States. https://doi.org/10.1038/s41467-018-03200-4. https://www.osti.gov/servlets/purl/1470638.
@article{osti_1470638,
title = {Route to high-energy density polymeric nitrogen t-N via He-N compounds},
author = {Li, Yinwei and Feng, Xiaolei and Liu, Hanyu and Hao, Jian and Redfern, Simon A. T. and Lei, Weiwei and Liu, Dan and Ma, Yanming},
abstractNote = {Polymeric nitrogen, stabilized by compressing pure molecular nitrogen, has yet to be recovered to ambient conditions, precluding its application as a high-energy density material. Here we suggest a route for synthesis of a tetragonal polymeric nitrogen, denoted t-N, via He-N compounds at high pressures. Using first-principles calculations with structure searching, we predict a class of nitrides with stoichiometry HeN4 that are energetically stable (relative to a mixture of solid He and N2) above 8.5 GPa. At high pressure, HeN4 comprises a polymeric channel-like nitrogen framework filled with linearly arranged helium atoms. The nitrogen framework persists to ambient pressure on decompression after removal of helium, forming pure polymeric nitrogen, t-N. t-N is dynamically and mechanically stable at ambient pressure with an estimated energy density of ~11.31 kJ/g, marking it out as a remarkable high-energy density material. As a result, this expands the known polymeric forms of nitrogen and indicates a route to its synthesis.},
doi = {10.1038/s41467-018-03200-4},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Mon Feb 19 00:00:00 EST 2018},
month = {Mon Feb 19 00:00:00 EST 2018}
}
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Fig. 1 : Thermodynamic stability of the predicted structures. Results from structure searching at 0 (a), 25 (b) and 50 (c) GPa. Convex hulls are shown as continuous lines, with (red) and without (black) the inclusion of vdW corrections. hcp-He at 0, 25 and 50 GPa, α-N2 at 0 GPamore »
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