Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Route to high-energy density polymeric nitrogen t-N via He-N compounds

Journal Article · · Nature Communications
 [1];  [2];  [3];  [1];  [4];  [5];  [5];  [6]
  1. Jiangsu Normal Univ., Xuzhou (China)
  2. Jilin Univ., Changchun (China); Univ. of Cambridge, Cambridge (United Kingdom)
  3. Carnegie Inst. of Washington, Washington, D.C. (United States)
  4. Univ. of Cambridge, Cambridge (United Kingdom); Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
  5. Deakin Univ., Waurn Ponds, VIC (Australia)
  6. Jilin Univ., Changchun (China)
+ Show Author Affiliations
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.
Research Organization:
Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Energy Frontier Research in Extreme Environments (EFree)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
NA0002006; SC0001057
OSTI ID:
1470638
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (60)

N 8 − Polynitrogen Stabilized on Multi-Wall Carbon Nanotubes for Oxygen-Reduction Reactions at Ambient Conditions journal August 2014
N 8 − Polynitrogen Stabilized on Multi-Wall Carbon Nanotubes for Oxygen-Reduction Reactions at Ambient Conditions journal August 2014
CALYPSO: A method for crystal structure prediction journal October 2012
High pressure X-ray diffraction study of potassium azide journal June 2011
Structural and electronic properties of sodium azide at high pressure: A first principles study journal May 2013
A New Allotrope of Nitrogen as High-Energy Density Material journal April 2016
Crystalline LiN 5 Predicted from First-Principles as a Possible High-Energy Material journal June 2015
A high-pressure van der Waals compound in solid nitrogen-helium mixtures journal July 1992
Calculations predict a stable molecular crystal of N8 journal December 2013
Reactions of xenon with iron and nickel are predicted in the Earth's inner core journal April 2014
A stable compound of helium and sodium at high pressure journal February 2017
Single-bonded cubic form of nitrogen journal July 2004
Synthesis of an open-framework allotrope of silicon journal November 2014
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets journal May 2021
Lead palladium titanate: A room temperature nanoscale multiferroic thin film journal February 2020
Pressure-induced planar N6 rings in potassium azide journal March 2014
Pressure-stabilized superconductive yttrium hydrides journal May 2015
A new high-pressure polymeric nitrogen phase in potassium azide journal January 2015
N 2 H: a novel polymeric hydronitrogen as a high energy density material journal January 2015
High P-T transformations of nitrogen to 170GPa journal May 2007
Highly repulsive interaction in novel inclusion D 2 –N 2 compound at high pressure: Raman and x-ray evidence journal January 2011
Structures and phase diagrams of N 2 and CO to 13 GPa by x‐ray diffraction journal March 1986
High pressure x‐ray diffraction studies on solid N 2 up to 43.9 GPa journal December 1990
Polymeric nitrogen conference January 1994
Polymerization of nitrogen in lithium azide journal October 2013
The metallization and superconductivity of dense hydrogen sulfide journal May 2014
Superconductive sodalite-like clathrate calcium hydride at high pressures journal April 2012
A nitrogen-rich C 3 N 12 solid transformed from cyanuric triazide under high pressure and temperature journal November 2010
Structure of Solid Helium by Neutron Diffraction journal January 1958
Polymeric nitrogen journal December 1992
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Vibrational line broadening in the mixed solid N 2 – Kr :   A high-pressure Raman study of the phase diagram journal October 2001
Density-functional study of nonmolecular phases of nitrogen: Metastable phase at low pressure journal July 2003
Low-pressure metastable phase of single-bonded polymeric nitrogen from a helical structure motif and first-principles calculations journal April 2007
First-principles calculations of the ferroelastic transition between rutile-type and CaCl 2 -type SiO 2 at high pressures journal October 2008
Crystal structure prediction via particle-swarm optimization journal September 2010
Structural and vibrational properties of the van der Waals compound (N 2 ) 11 He up to 135 GPa journal April 2011
Van der Waals density functionals applied to solids journal May 2011
Stable structures of He and H 2 O at high pressure journal January 2015
Dissociation products and structures of solid H 2 S at strong compression journal January 2016
Novel High Pressure Structures of Polymeric Nitrogen journal February 2009
High-Pressure Phases of Nitrogen journal March 2009
Efficient Implementation of a van der Waals Density Functional: Application to Double-Wall Carbon Nanotubes journal August 2009
Predicted Novel High-Pressure Phases of Lithium journal January 2011
Substitutional Alloy of Bi and Te at High Pressure journal April 2011
Cagelike Diamondoid Nitrogen at High Pressures journal October 2012
Stable All-Nitrogen Metallic Salt at Terapascal Pressures journal October 2013
High Energy Density Mixed Polymeric Phase from Carbon Monoxide and Nitrogen journal December 2013
Pressure-Induced Symmetry-Lowering Transition in Dense Nitrogen to Layered Polymeric Nitrogen (LP-N) with Colossal Raman Intensity journal November 2014
High-Energy Density and Superhard Nitrogen-Rich B-N Compounds journal September 2015
Van der Waals Density Functional for General Geometries journal June 2004
Prediction of New Phases of Nitrogen at High Pressure from First-Principles Simulations journal September 2004
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data journal October 2011
Electron diffraction and the structure of α-N 2 journal April 1974
Novel high-pressure phase with pseudo-benzene “N 6 ” molecule of LiN 3 journal January 2013
Pressure-induced polymerization of nitrogen in potassium azides journal October 2013
Van der Waals density functionals applied to solids text January 2011
CALYPSO: a method for crystal structure prediction text January 2012
Phases of HeN4 and polymeric nitrogen t-N as a function of pressure dataset January 2017

Cited By (23)

Structurally uneasy but kinetically stable nitrogens in 1,3‐disubstituted cyclotetrazenes: Viable high‐energy‐density materials journal May 2019
Multiple superionic states in helium–water compounds journal July 2019
Multifold pressure-induced increase of electric conductivity in LiFe0.75V0.10PO4 glass journal November 2019
Carbon network evolution from dimers to sheets in superconducting ytrrium dicarbide under pressure journal November 2018
Electrostatic force driven helium insertion into ammonia and water crystals under pressure journal September 2019
A kinetically persistent isomer found for pentazole: a global potential energy surface survey journal January 2019
Effect of pressure on the structural, electronic and mechanical properties of ultraincompressible W 2 B journal January 2018
Origin of the considerably high thermal stability of cyclo-N 5 − containing salts at ambient conditions journal January 2019
Beyond molecular nitrogen: revelation of two ambient-pressure metastable single- and double-bonded nitrogen allotropes built from three-membered rings journal January 2019
Armchair shaped polymeric nitrogen N 8 chains confined in h-BN matrix at ambient conditions: stability and vibration analysis journal January 2019
Prediction of pressure-induced phase transformations in Mg 3 As 2 journal January 2019
Prediction of superhard B 2 N 3 with two-dimensional metallicity journal January 2019
Prediction of strain-induced phonon-mediated superconductivity in monolayer YS journal January 2019
Ti-fraction-induced electronic and magnetic transformations in titanium oxide films journal April 2019
Mixed cationic clusters of nitrogen and hydrogen journal January 2020
High-pressure modulated structures in beryllium chalcogenides journal July 2019
Effect of covalent bonding on the superconducting critical temperature of the H-S-Se system journal November 2018
Rare Helium-Bearing Compound FeO 2 He Stabilized at Deep-Earth Conditions journal December 2018
Exploring the structural, mechanical, thermodynamic, and electronic properties of (Ni 0.66 , Zn 0.33 ) 3 Sn 4 ternary intermetallic compounds by the first-principles study journal January 2020
Carbon network evolution from dimers to sheets in superconducting ytrrium dicarbide under pressure text January 2018
Multiple superionic states in helium–water compounds text January 2019
High-pressure modulated structures in beryllium chalcogenides text January 2019
Electrostatic force driven helium insertion into ammonia and water crystals under pressure text January 2019

Figures / Tables (5)

Fig. 1(p. 3)figure Fig. 1
Fig. 2(p. 4)figure Fig. 2
Fig. 3(p. 5)figure Fig. 3
Fig. 4(p. 5)figure Fig. 4
Table 1(p. 5)table Table 1

Similar Records

Polymerization of nitrogen in cesium azide under modest pressure
Journal Article · Mon Jul 28 00:00:00 EDT 2014 · Journal of Chemical Physics · OSTI ID:22419963
Exotic stable cesium polynitrides at high pressure
Journal Article · Wed Nov 18 19:00:00 EST 2015 · Scientific Reports · OSTI ID:1241100
Polymeric nitrogen
Journal Article · Mon Nov 30 23:00:00 EST 1992 · Physical Review, B: Condensed Matter; (United States) · OSTI ID:6958714

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
catalysis (heterogeneous)
charge transport
energy storage (including batteries and capacitors)
hydrogen and fuel cells
materials and chemistry by design
mesostructured materials
phonons
solar (photovoltaic)
superconductivity
synthesis (novel materials)
thermoelectric