Vibrational Dynamics and Phase Transitions of Hydrazine to 50 GPa

Ripani, Roma; Gramsch, Stephen A.; Safari, Fatemeh; Ahart, Muhtar; Liu, Zhenxian; Dattelbaum, Dana M.; Hemley, Russell J.

doi:10.1021/acsomega.4c09047

Vibrational Dynamics and Phase Transitions of Hydrazine to 50 GPa

Journal Article · Fri Feb 21 00:00:00 EST 2025 · ACS Omega

DOI:https://doi.org/10.1021/acsomega.4c09047· OSTI ID:2520575

^[1]; Gramsch, Stephen A. ^[1]; ^[1]; Ahart, Muhtar ^[1]; Liu, Zhenxian ^[1]; Dattelbaum, Dana M. ^[2]; ^[1]

University of Illinois, Chicago, IL (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

The high pressure behavior of hydrazine, N₂H₄, has been investigated to 50 GPa at room temperature using infrared and Raman spectroscopy to explore pressure induced phase transitions and changes in hydrogen bonding. Three solid–solid phase transitions were detected at 11, 21, and 32 GPa on room temperature compression through dramatic changes in the lattice vibration and N–H stretching regions with increasing pressure in both measurement techniques. The transition to phase IV, which appears at 32 GPa, exhibits increased hydrogen bonding with significant hysteresis, persisting to 9 GPa on decompression. This work presents a detailed analysis of the pressure dependence of mode shifts and calculations of mode Grüneisen parameters as well as a determination of an approximate thermodynamic Grüneisen parameter. We compare these results to the behavior of other small molecular materials such as ammonia and water and explore the evolution of hydrogen bonding in hydrazine toward the symmetrically hydrogen bonded state, which has previously been suggested by theoretical computations.

View Journal Article

Research Organization:: University of Illinois, Chicago, IL (United States)

Sponsoring Organization:: Army Research Office (ARO); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: NA0003975; NA0004153; SC0012704

OSTI ID:: 2520575

Alternate ID(s):: OSTI ID: 2549404
OSTI ID: 2527246

Journal Information:: ACS Omega, Journal Name: ACS Omega Journal Issue: 8 Vol. 10; ISSN 2470-1343

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (42)

Raman spectra of gases. XV: Hydrazine and hydrazine-d4 Durig, J. R.; Griffin, M. G.; Macnamee, R. W. Journal of Raman Spectroscopy, Vol. 3, Issue 2-3 https://doi.org/10.1002/jrs.1250030204	journal	April 1975
Direct hydrazine fuel cells: A review Serov, Alexey; Kwak, Chan Applied Catalysis B: Environmental, Vol. 98, Issue 1-2 https://doi.org/10.1016/j.apcatb.2010.05.005	journal	July 2010
Hydrazine at high pressure Pravica, Michael; Bai, Ligang; Liu, Yu Chemical Physics Letters, Vol. 555 https://doi.org/10.1016/j.cplett.2012.10.079	journal	January 2013
Synthesis of Atomically Thin Hexagonal Diamond with Compression Ke, Feng; Zhang, Lingkong; Chen, Yabin Nano Letters, Vol. 20, Issue 8 https://doi.org/10.1021/acs.nanolett.0c01872	journal	June 2020
High Pressure Study of Ru ₃ (CO) ₁₂ by X-ray Diffraction, Raman, and Infrared Spectroscopy Slebodnick, Carla; Zhao, Jing; Angel, Ross Inorganic Chemistry, Vol. 43, Issue 17 https://doi.org/10.1021/ic049617y	journal	August 2004
New phases and chemical reactions in solid carbon monoxide under pressure Katz, Allen I.; Schiferl, David; Mills, Robert L. The Journal of Physical Chemistry, Vol. 88, Issue 15 https://doi.org/10.1021/j150659a007	journal	July 1984
The Heats of Combustion of Some Nitrogen Compounds and the Apparent Energy of the N-N Bond ^1a,b Cole, Leland G.; Gilbert, E. C. Journal of the American Chemical Society, Vol. 73, Issue 11 https://doi.org/10.1021/ja01155a120	journal	November 1951
Dihydrogen Bonding under High Pressure: A Raman Study of BH₃NH₃ Molecular Crystal Custelcean, Radu; Dreger, Zbigniew A. The Journal of Physical Chemistry B, Vol. 107, Issue 35 https://doi.org/10.1021/jp035267+	journal	August 2003
Hydrogen Bond in Compressed Solid Hydrazine Jiang, Shuqing; Huang, Xiaoli; Duan, Defang The Journal of Physical Chemistry C, Vol. 118, Issue 6 https://doi.org/10.1021/jp4102543	journal	January 2014
Pressure-Induced Phase Transition in N–H···O Hydrogen-Bonded Molecular Crystal Biurea: Combined Raman Scattering and X-ray Diffraction Study Yan, Tingting; Wang, Kai; Tan, Xiao The Journal of Physical Chemistry C, Vol. 118, Issue 28 https://doi.org/10.1021/jp503803n	journal	July 2014
Compression and Probing C−H···I Hydrogen Bonds of Iodoform under High Pressure by X-ray Diffraction and Raman Scattering Liu, Dan; Lei, Weiwei; Wang, Kai The Journal of Physical Chemistry B, Vol. 113, Issue 21 https://doi.org/10.1021/jp900467z	journal	April 2009
Calibration of the ruby pressure gauge to 800 kbar under quasi-hydrostatic conditions Mao, H. K.; Xu, J.; Bell, P. M. Journal of Geophysical Research, Vol. 91, Issue B5, p. 4673-4676 https://doi.org/10.1029/JB091iB05p04673	journal	January 1986
Pressure-induced chemistry in a nitrogen-hydrogen host–guest structure Spaulding, Dylan K.; Weck, Gunnar; Loubeyre, Paul Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6739	journal	December 2014
High-energy-density extended CO solid Lipp, Magnus J.; Evans, William J.; Baer, Bruce J. Nature Materials, Vol. 4, Issue 3 https://doi.org/10.1038/nmat1321	journal	February 2005
Ab Initio Prediction of the Phase Transition for Solid Ammonia at High Pressures Huang, Lei; Han, Yanqiang; Liu, Jinyun Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-64030-3	journal	May 2020
Nitrogen Backbone Oligomers Wang, Hongbo; Eremets, Mikhail I.; Troyan, Ivan Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep13239	journal	August 2015
Pressure-induced chemical reactions in the N ₂ (H ₂ ) ₂ compound: from the N ₂ and H ₂ species to ammonia and back down into hydrazine Laniel, D.; Svitlyk, V.; Weck, G. Physical Chemistry Chemical Physics, Vol. 20, Issue 6 https://doi.org/10.1039/C7CP07989C	journal	January 2018
On the Infrared Spectrum of Hydrazine Giguère, Paul A.; Liu, I. D. The Journal of Chemical Physics, Vol. 20, Issue 1 https://doi.org/10.1063/1.1700155	journal	January 1952
Far-Infrared Spectra and Space Group of Crystalline Hydrazine and Hydrazine-d4 Baglin, F. G.; Bush, S. F.; Durig, J. R. The Journal of Chemical Physics, Vol. 47, Issue 6 https://doi.org/10.1063/1.1712242	journal	September 1967
Structural transformation of molecular nitrogen to a single-bonded atomic state at high pressures Eremets, M. I.; Gavriliuk, A. G.; Serebryanaya, N. R. The Journal of Chemical Physics, Vol. 121, Issue 22 https://doi.org/10.1063/1.1814074	journal	January 2004
Optical and Raman Microspectroscopy of Nitrogen and Hydrogen Mixtures at high Pressures Ciezak, Jennifer A.; Jenkins, Timothy A.; Hemley, Russell J. SHOCK COMPRESSION OF CONDENSED MATTER 2009: Proceedings of the American Physical Society Topical Group on Shock Compression of Condensed Matter, AIP Conference Proceedings https://doi.org/10.1063/1.3295042	conference	January 2009
The effect of pressure on the Raman spectrum of NH4I Heyns, A. M.; Hirsch, K. R.; Holzapfel, W. B. The Journal of Chemical Physics, Vol. 73, Issue 1 https://doi.org/10.1063/1.439904	journal	July 1980
Backbone NxH compounds at high pressures Goncharov, Alexander F.; Holtgrewe, Nicholas; Qian, Guangrui The Journal of Chemical Physics, Vol. 142, Issue 21 https://doi.org/10.1063/1.4922051	journal	June 2015
The high-pressure dimension in earth and planetary science Mao, H. -k.; Hemley, R. J. Proceedings of the National Academy of Sciences, Vol. 104, Issue 22 https://doi.org/10.1073/pnas.0703653104	journal	May 2007
The symmetry groups of non-rigid molecules Longuet-Higgins, H. C. Molecular Physics, Vol. 6, Issue 5 https://doi.org/10.1080/00268976300100501	journal	June 1963
The Unexpected Stability of Hydrazine Molecules in Hydrous Environment under Pressure* Jiang, Shu-Qing; Yang, Xue; Huang, Xiao-Li Chinese Physics Letters, Vol. 37, Issue 1 https://doi.org/10.1088/0256-307X/37/1/016102	journal	January 2020
A high-pressure study of PbCO ₃ by XRD and Raman spectroscopy Zhang, Yu-Feng; Liu, Jing; Qin, Zhen-Xing Chinese Physics C, Vol. 37, Issue 3 https://doi.org/10.1088/1674-1137/37/3/038001	journal	March 2013
High pressure spectroscopic studies of hydrazine (N ₂ H ₄ ) Chellappa, Raja; Dattelbaum, Dana; Daemen, Luke Journal of Physics: Conference Series, Vol. 500, Issue 5 https://doi.org/10.1088/1742-6596/500/5/052008	journal	May 2014
High-pressure elastic properties of liquid and solid ammonia Kume, T.; Daimon, M.; Sasaki, S. Physical Review B, Vol. 57, Issue 21 https://doi.org/10.1103/PhysRevB.57.13347	journal	June 1998
High-pressure spectroscopic investigation of multiferroic Ni 3 TeO 6 O'Neal, Kenneth R.; Clune, Amanda J.; Harms, Nathan C. Physical Review B, Vol. 98, Issue 18 https://doi.org/10.1103/PhysRevB.98.184101	journal	November 2018
Synchrotron Infrared Measurements of Dense Hydrogen to 360 GPa Zha, Chang-Sheng; Liu, Zhenxian; Hemley, Russell J. Physical Review Letters, Vol. 108, Issue 14 https://doi.org/10.1103/PhysRevLett.108.146402	journal	April 2012
Reactivity of Hydrogen-Helium and Hydrogen-Nitrogen Mixtures at High Pressures Turnbull, Robin; Donnelly, Mary-Ellen; Wang, Mengnan Physical Review Letters, Vol. 121, Issue 19 https://doi.org/10.1103/PhysRevLett.121.195702	journal	November 2018
Pressure-Induced Collapse of Magnetic Order in Jarosite Klein, Ryan A.; Walsh, James P. S.; Clarke, Samantha M. Physical Review Letters, Vol. 125, Issue 7 https://doi.org/10.1103/PhysRevLett.125.077202	journal	August 2020
Fityk : a general-purpose peak fitting program Wojdyr, Marcin Journal of Applied Crystallography, Vol. 43, Issue 5 https://doi.org/10.1107/S0021889810030499	journal	September 2010
The crystal structure of hydrazine Collin, R. L.; Lipscomb, W. N. Acta Crystallographica, Vol. 4, Issue 1 https://doi.org/10.1107/S0365110X51000027	journal	January 1951
Crystal structure prediction and hydrogen-bond symmetrization of solid hydrazine under high pressure: a first-principles study Zhang, Hua-Di; Zheng, Song-Kuan; Jin, Xi-Lian Acta Crystallographica Section C Structural Chemistry, Vol. 70, Issue 2 https://doi.org/10.1107/S2053229613032324	journal	January 2014
Crystal Structure of the High-Pressure Phase of Solid CO2 Aoki, K.; Yamawaki, H.; Sakashita, M. Science, Vol. 263, Issue 5145 https://doi.org/10.1126/science.263.5145.356	journal	January 1994
Compression of Ice to 210 Gigapascals: Infrared Evidence for a Symmetric Hydrogen-Bonded Phase Goncharov, A. F.; Struzhkin, V. V.; Somayazulu, M. S. Science, Vol. 273, Issue 5272 https://doi.org/10.1126/science.273.5272.218	journal	July 1996
Quartzlike Carbon Dioxide: An Optically Nonlinear Extended Solid at High Pressures and Temperatures Iota, V. Science, Vol. 283, Issue 5407 https://doi.org/10.1126/science.283.5407.1510	journal	March 1999
Raman Spectroscopy at High Pressures Goncharov, Alexander F. International Journal of Spectroscopy, Vol. 2012 https://doi.org/10.1155/2012/617528	journal	January 2012
Thermodynamic properties of hydrazine. Haws, Jimmy L.; Harden, Barrel G. Journal of Spacecraft and Rockets, Vol. 2, Issue 6 https://doi.org/10.2514/3.28327	journal	November 1965
High-Pressure Raman and Infrared Spectroscopic Study of Prehnite Ross, Nancy L.; Detrie, Theresa A.; Liu, Zhenxian Minerals, Vol. 10, Issue 4 https://doi.org/10.3390/min10040312	journal	March 2020

Similar Records

Structural stability, dihydrogen bonding, and pressure-induced polymorphic transformations in hydrazine borane

Journal Article · Thu Jul 13 20:00:00 EDT 2023 · Physical Chemistry Chemical Physics. PCCP · OSTI ID:2423652

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Compression
Infrared light
Noncovalent interactions
Phase transitions
Raman spectroscopy

Vibrational Dynamics and Phase Transitions of Hydrazine to 50 GPa

Citation Formats

References (42)

Similar Records

Related Subjects