Route to Stabilize Cubic Gauche Polynitrogen to Ambient Conditions via Surface Saturation by Hydrogen
Guo Chen1,2† , Caoping Niu1,2† , Wenming Xia1,2 , Jie Zhang1 , Zhi Zeng1,2 , and Xianlong Wang1,2*
1 Key Laboratory of Materials Physics, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, China2 University of Science and Technology of China, Hefei 230026, China
Abstract ：Cubic gauche polynitrogen (cg-N) is an attractive high-energy density material. However, high-pressure synthesized cg-N will decompose at low pressure and cannot exist under ambient conditions. Here, the stabilities of cg-N surfaces with and without saturations at different pressures and temperatures are systematically investigated based on first-principles calculations and molecular dynamics simulations. Pristine surfaces at 0 GPa are very brittle and will decompose at 300 K, especially (110) surface will collapse completely just after structural relaxation, whereas the decompositions of surfaces can be suppressed by applying pressure, indicating that surface instability causes the cg-N decomposition at low pressure. Due to the saturation of dangling bonds and transferring electrons to the surfaces, saturation with H can stabilize surfaces under ambient conditions, while it is impossible for OH saturation to occur solely from obtaining electrons from surfaces. This suggests that polynitrogen is more stable in an acidic environment or when the surface is saturated with less electronegative adsorbates.
收稿日期: 2023-05-25
Express Letter
出版日期: 2023-07-22
PACS:
61.50.Ah
(Theory of crystal structure, crystal symmetry; calculations and modeling)
62.50.-p
(High-pressure effects in solids and liquids)
68.35.-p
(Solid surfaces and solid-solid interfaces: structure and energetics)
68.35.Md
(Surface thermodynamics, surface energies)
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2023, Vol. 40 
