Pressure-induced polymerization of P(CN) 3

Gou, Huiyang; Yonke, Brendan L.; Epshteyn, Albert; Kim, Duck Young; Smith, Jesse S.; Strobel, Timothy A.

doi:10.1063/1.4919640

Pressure-induced polymerization of P(CN) ₃

Journal Article · Thu May 21 00:00:00 EDT 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4919640· OSTI ID:1338321

^[1]; Yonke, Brendan L. ^[2]; Epshteyn, Albert ^[2]; Kim, Duck Young ^[3]; Smith, Jesse S. ^[3]; Strobel, Timothy A. ^[3]

Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab.; Carnegie Institution of Washington
Naval Research Lab. (NRL), Washington, DC (United States)
Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab.

Motivated to explore the formation of novel extended carbon-nitrogen solids via well-defined molecular precursor pathways, we studied the chemical reactivity of highly pure phosphorous tricyanide, P(CN)₃, under conditions of high pressure at room temperature. Raman and infrared (IR) spectroscopic measurements reveal a series of phase transformations below 10 GPa, and several low-frequency vibrational modes are reported for the first time. Synchrotron powder Xray diffraction (PXRD) measurements taken during compression show that molecular P(CN)₃ is highly compressible with a bulk modulus of 10.0±0.3 GPa and polymerizes into an amorphous solid above ~10.0 GPa. Raman and infrared (IR) spectra, together with first-principles molecular-dynamics simulations, show that the amorphization transition is associated with polymerization of the cyanide groups into CN bonds with predominantly sp² character, similar to known carbon nitrides, resulting in a novel PCN polymeric phase, which is recoverable to ambient pressure.

View Accepted Manuscript (DOE)

Research Organization:: Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab.

Sponsoring Organization:: USDOE; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-06CH11357; FG02-99ER45775; NA0001974; NA0002006

OSTI ID:: 1338321

Alternate ID(s):: OSTI ID: 1228173
OSTI ID: 22415804
OSTI ID: 1182777

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 19 Vol. 142; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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