Backbone NxH compounds at high pressures
Abstract
Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first principles theoretical structure predictions to investigate mixtures of N2 and H2 up to 55 GPa. Our experiments show the formation of structurally complex van der Waals compounds above 10 GPa. However, we found that these NxH (0.5<1.5) compounds transform abruptly to new oligomeric materials through barochemistry above 47 GPa and photochemistry at pressures as low as 10 GPa. These oligomeric compounds can be recovered to ambient pressure at T<130 K, whereas at room temperature, they can be metastable on pressure release down to 3.5 GPa. Extensive theoretical calculations show that such oligomeric materials become thermodynamically more stable in comparison to mixtures of N2, H2, and NH3 above approximately 40 GPa. Lastly, our results suggest new pathways for synthesis of environmentally benign high energy-density materials. These materials could also exist as alternative planetary ices.
- Authors:
-
- Chinese Academy of Sciences (CAS), Anhui (China); Carnegie Institution of Washington, Washington, D.C. (United States); Univ. of Science and Technology of China, Hefei (China)
- Carnegie Institution of Washington, Washington, D.C. (United States); Howard Univ., Washington, D.C. (United States)
- State Univ. of New York, Stony Brook, NY (United States); Guilin Univ. of Electronic Technology, Guilin (China)
- Guilin Univ. of Electronic Technology, Guilin (China)
- Skolkovo Institute of Science and Technology, Moscow (Russia); State Univ. of New York, Stony Brook, NY (United States); Guilin Univ. of Electronic Technology, Guilin (China); Moscow Institute of Physics and Technology, Moscow Region (Russian Federation)
- Carnegie Institution of Washington, Washington, D.C. (United States)
- Univ. College London, London (United Kingdom)
- Chinese Academy of Sciences (CAS), Anhui (China)
- Howard Univ., Washington, D.C. (United States)
- Carnegie Institution of Washington, Washington, D.C. (United States); V.S. Sobolev Institute of Geology and Mineralogy, Novosibirsk (Russia)
- Deutsches Elektronen-Synchrotron (DESY) Photon Science, Hamburg (Germany)
- Univ. of Chicago, Chicago, IL (United States)
- Publication Date:
- Research Org.:
- Carnegie Institution of Washington, Washington, D.C. (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1335451
- Alternate Identifier(s):
- OSTI ID: 1228626
- Grant/Contract Number:
- NA0002006; AC02-98CH10086; FG02-94ER14466
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 21; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Goncharov, Alexander F., Holtgrewe, Nicholas, Qian, Guangrui, Hu, Chaohao, Oganov, Artem R., Somayazulu, Maddury, Stavrou, Elissaios, Pickard, Chris J., Berlie, Adam, Yen, Fei, Mahmood, Mahmood, Lobanov, Sergey S., Konopkova, Zuzana, and Prakapenka, Vitali B. Backbone NxH compounds at high pressures. United States: N. p., 2015.
Web. doi:10.1063/1.4922051.
Goncharov, Alexander F., Holtgrewe, Nicholas, Qian, Guangrui, Hu, Chaohao, Oganov, Artem R., Somayazulu, Maddury, Stavrou, Elissaios, Pickard, Chris J., Berlie, Adam, Yen, Fei, Mahmood, Mahmood, Lobanov, Sergey S., Konopkova, Zuzana, & Prakapenka, Vitali B. Backbone NxH compounds at high pressures. United States. https://doi.org/10.1063/1.4922051
Goncharov, Alexander F., Holtgrewe, Nicholas, Qian, Guangrui, Hu, Chaohao, Oganov, Artem R., Somayazulu, Maddury, Stavrou, Elissaios, Pickard, Chris J., Berlie, Adam, Yen, Fei, Mahmood, Mahmood, Lobanov, Sergey S., Konopkova, Zuzana, and Prakapenka, Vitali B. Fri .
"Backbone NxH compounds at high pressures". United States. https://doi.org/10.1063/1.4922051. https://www.osti.gov/servlets/purl/1335451.
@article{osti_1335451,
title = {Backbone NxH compounds at high pressures},
author = {Goncharov, Alexander F. and Holtgrewe, Nicholas and Qian, Guangrui and Hu, Chaohao and Oganov, Artem R. and Somayazulu, Maddury and Stavrou, Elissaios and Pickard, Chris J. and Berlie, Adam and Yen, Fei and Mahmood, Mahmood and Lobanov, Sergey S. and Konopkova, Zuzana and Prakapenka, Vitali B.},
abstractNote = {Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first principles theoretical structure predictions to investigate mixtures of N2 and H2 up to 55 GPa. Our experiments show the formation of structurally complex van der Waals compounds above 10 GPa. However, we found that these NxH (0.5<1.5) compounds transform abruptly to new oligomeric materials through barochemistry above 47 GPa and photochemistry at pressures as low as 10 GPa. These oligomeric compounds can be recovered to ambient pressure at T<130 K, whereas at room temperature, they can be metastable on pressure release down to 3.5 GPa. Extensive theoretical calculations show that such oligomeric materials become thermodynamically more stable in comparison to mixtures of N2, H2, and NH3 above approximately 40 GPa. Lastly, our results suggest new pathways for synthesis of environmentally benign high energy-density materials. These materials could also exist as alternative planetary ices.},
doi = {10.1063/1.4922051},
journal = {Journal of Chemical Physics},
number = 21,
volume = 142,
place = {United States},
year = {Fri Jun 05 00:00:00 EDT 2015},
month = {Fri Jun 05 00:00:00 EDT 2015}
}
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