Route to Stabilize Cubic Gauche Polynitrogen to Ambient Conditions via Surface Saturation by Hydrogen
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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. -
The triple bond in nitrogen molecule (N≡N with bonding energy of 954 kJ/mol) is one of the strongest chemical bonds of all molecules, and the bonding energy will be decrease and total energy will increase significantly if the N≡N is transformed into the double bond (N=N with bonding energy of 418 kJ/mol) and the single bond (N–N with bonding energy of 160 kJ/mol).[1] On the other hand, an enormous amount of energy will be released when the N–N and N=N decompose into the N≡N. Therefore, polymerized nitrogen containing N–N or N=N has been attracted lots of interests for potential applications as high-energy density material (HEDM).[2–26]
To break N≡N and synthesize polymerized nitrogen, extreme synthetic conditions are needed, and high pressure is a popular way.[27] Existing works have shown that within the low pressure range, nitrogen exists in the form of molecule crystals.[28–33] The first polymerized nitrogen with fully single bonding, named as cubic gauche polynitrogen (cg-N), was theoretically predicted to appear at 50 GPa,[29] and its energy density is about five times larger than that of TNT.[34] Furthermore, many kinds of polynitrogens (such as chains,[35,36] layers,[37,38] cage,[39] and polynitrogen[40,41]) were theoretically proposed to be thermodynamically stable at high pressure. In 2004, the cg-N was successfully synthesized under the extreme conditions of 110 GPa and 2000 K.[42] Following cg-N, layered polymeric nitrogen (LP-N),[43] black phosphorus nitrogen (BP-N),[44] and hexagonal layered polymeric nitrogen (HLP-N)[45] have been synthesized at the pressures of 120 GPa, 150 GPa, and 180 GPa, respectively. Nevertheless, the synthetic pressure of cg-N is the smallest among these synthesized polymeric all-nitrogen materials.
Importantly, there are nonnegative frequencies in the phonon spectra of cg-N at 0 GPa,[46] indicating that it potentially can be quenched to the ambient pressure. However, the cg-N becomes unstable and begins to decompose with pressure decreasing to 42 GPa at room temperature or to 25 GPa at temperature of 140 K,[42] and the same phenomenon also occurs to other polymeric all-nitrogen materials. For example, LP-N, HLP-N, and BP-N can only be stabilized up to 52 GPa, 66 GPa, and 48 GPa at room temperature, respectively,[43–45] which hinder their practical applications as HEDMs. In order to preserve cg-N to the ambient pressure, at present, the important tasks are to find out its decomposition mechanism at low pressure and to find a way to stabilize it under ambient conditions.
It is generally believed that decomposition of materials will start from the weakest bonds, which may exist on the surfaces containing energy unfavorable dangling bonds.[47] A typical example is that reconstructions are usually observed on materials’ surfaces because of the instability of free surfaces, such as Au (111) and Si (100).[48,49] The weakest bond of cg-N may also exist on the surface. Actually, the stability is improved when the cg-N is placed in the carbon nanotubes, indicating that surface stability may strongly affect the stability of cg-N.[50] However, so far, the surface stabilities of cg-N have not been well illustrated.
In this work, we investigate the stabilities of cg-N low-index surfaces at different pressures (0 GPa, 40 GPa, 80 GPa, 100 GPa, 120 GPa) under different saturated conditions (H, OH, CH3), using the first-principles method as implemented in the Vienna ab initio approximation package (VASP) combined with molecular dynamics (MD) method. Our results show that the instabilities of pristine surfaces cause the cg-N decomposition at low pressure. The saturation of OH cannot improve the surface stabilities, while all investigated surfaces can be stabilized under ambient conditions by H-saturation due to the electron transform from H to surfaces.
The crystal structure of cg-N is shown in Fig. S1(a) in the Supplementary Materials, where the local coordination environments of N is similar to that of NH3. Each N atom connects with other three neighbors via N–N single bonds, and two electrons form a lone pair of electrons. The N–N single bonds are connected to each other, forming a cubic gauche configuration.[29] All sub-surfaces obtained from the Miller indices of (100), (110), and (111) are shown in Figs. S1(b)–S1(h). By exposing different surfaces to vacuum, two [(100a), (100b)] and four [(110a), (110b), (110c), (110d)] kinds of surfaces are constructed based on the Miller indices of (100) and (110), respectively, and only one surface (111a) is obtained in the case of (111) Miller indices. The corresponding free surfaces constructed are shown in Fig. S2(a).
The configurations of pristine surfaces after structural relaxation at 0 GPa are shown in Fig. 1(a). The (100a) and (111a) surfaces are stable, keeping their original structures, while linear N3 groups (similar to the azide ion) are formed and adsorbed on (110c) surface, giving rise to a stable reconfigured (110c) [i.e., r-(110c)] surface. After releasing one nitrogen molecule, the (100b) surface transfers to the stable (100a) surface. Similar phenomenon occurs in the (110a) surface, and it will transfer to the r-(110c) surface after releasing two nitrogen molecules. Interestingly, the (110b) surface breaks down layer by layer via releasing nitrogen molecules and decomposes completely under the processes of structure relaxation. The (110d) surface is also dissociative completely as well, breaking down into zigzag nitrogen chains and nitrogen molecules. Therefore, the (110b) and (110d) surfaces are the weakest among those of all investigated sub-surfaces. In the following, we investigate the stability of (110b) and (110d) surfaces under high pressure.
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Fig. Fig. 1. Stabilities of pristine surfaces. (a) Structures of pristine surfaces after structural relaxations at 0 GPa. (b) Optimized structures of (110d) surfaces at pressures ranging from 0 GPa to 120 GPa, and He atoms are filled in vacuum zone. (c) Structures of pristine (100a), (110c), and (111a) surfaces after MD simulations at 300 K by using the supercell with 192 N atoms. The atoms located in the blue shadow area are fixed. For structural relaxations filled with He at high pressure, all nitrogen atoms and helium atoms are allowed to relax. To clearly show the atomic structure of surfaces, the vacuum between surfaces are not fully presented, and it is indicated by the dotted lines. Blue balls represent nitrogen atoms and orange represents helium atoms.To apply hydrostatic pressure on the surfaces, helium gas employed to fill the vacuum zone. The relaxed structures of (110d) surfaces at high pressure are shown in Fig. 1(b). We can find that at the pressures of 100 GPa and 120 GPa closed to the conditions of experimentally synthesized cg-N, the (110d) surface is stable. Furthermore, the structure is maintained with pressure decreasing to 60 GPa, and slight surface decomposition appears at 40 GPa and 20 GPa, and totally structural decomposition occurs at 0 GPa. As shown in Fig. S3 in the Supplementary Materials, the stability of (110b) surface is also significantly enhanced by applying high pressures larger than 20 GPa. The results agree well with experimental observations, where the cg-N can only be quenched to 25 GPa at low temperature.[42] Based on the above results, we can make the following assumption about the process of cg-N decomposition: Since pressure can enhance the stability of surfaces, the surface decompositions will be suppressed under high-pressure conditions, resulting in a stable cg-N, and surfaces eventually become unstable after depressurization, disintegrating the whole structure.
MD simulations were performed to study the stabilities of the (100a), (111a), and r-(110c) surfaces at 0 GPa and 300 K. To allow for sufficient relaxation of the surface, the supercell for MD simulation is increased 2 × 2 times as much as that used during structure relaxation. All subsequent MD simulations were conducted using this larger supercells. The corresponding z-axis mean square displacements (MSDs) are shown in Fig. S4. We can find that the MSDs of both (100a) and (111a) surfaces at 300 K increase noticeably, and corresponding N–N networks are broken down from surface after MD simulations [Fig. 1(c)], indicating that (100a) and (111a) surfaces cannot exist stably at 300 K. In contrast, the MSD of r-(110c) surface at 300 K is almost a constant, and its structure can exist stably. It is easier to stabilize cg-N at low temperatures, which is consistent with the previous experimental result.[42,51] The above results show that except r-(110c) surface, all investigated pristine surfaces are not stable under ambient conditions.
To stabilize the high-pressure synthesized cg-N under the ambient conditions and to promote its practical applications, it is necessary to find a way to stabilize the unstable surfaces [especially (110b) and (110d) surfaces], and to enhance the finite-temperature stabilities of all investigated surfaces. The high stability of r-(110c) surface, where the dangling bonds on the surface are saturated with the linear N3 groups, indicates that saturation of the dangling bonds is important for enhancing the stabilities of cg-N surfaces. Therefore, saturations of dangling bonds at 0 GPa with H, OH, and CH3 are investigated, and the corresponding saturated surfaces are named as surface-H, surface-OH, and surface-CH3, respectively (see Fig. S2 in the Supplementary Materials).
The stabilities of surfaces with (without) saturations under the static condition and at 300 K are summarized in Fig. 2. The OH saturation does not improve the surface stabilities, since the stabilities of (100b), (110d), and (111a) surfaces are enhanced but (100a) and r-(110c) surfaces changes from stable to unstable, while the others remains unchanged. Furthermore, the CH3 saturation provides finite stabilizing effect that all surfaces are improved except (100a)-CH3 surface, and three surfaces [(100b), (110b) and (110c)] cannot exist stably at 300 K. However, with H saturation, all investigated surfaces are stable at 300 K, indicating that the cg-N can be stabilized to ambient conditions if its surfaces are saturated with hydrogen. Please note that for two stable pristine surfaces [(100a) and (111a)], the H adsorption energies of (100a)-H and (111a)-H are −0.794 eV and −1.278 eV, respectively, and H saturation is an energy-favorable process.
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Fig. Fig. 2. The stabilities of surfaces without and with H, OH, and CH3 saturations after structure relaxation and MD simulations at 300 K. The brackets on the y-axis tags show the average number of electrons (in units of e) transferred from adsorbates to surface, where positive (negative) values present electrons transfer from adsorbates to surfaces (from surfaces to adsorbates). The r-(110c) means the (110c) surface with surface reconstruction. SR: structural relaxation.We further run MD simulations for surface-H at higher temperatures of 500 K, 750 K, 1000 K, and 1250 K for illustrating the maximum temperature that can be stabilized by H saturation, which is important for its practical application as HEDM. The corresponding z-axis MSD at temperatures before and after the structure loses stability, as shown in Fig. 3(a). We can find that H saturation can improve the stability of all surfaces to at least 750 K and even more than half of the surfaces [(100a), (100b), (110a) and (110d)] can be stabilized to 1000 K. The stabilities of surface-H are summarized in Fig. 3(b) including that of pristine surfaces used for comparison, indicating that H saturation can enhance the stabilities of cg-N surfaces significantly.
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Fig. Fig. 3. Stabilities of surfaces with H saturation. (a) The MSD of surface-H at the temperature before (blue line) and after (red line) structure collapse. (b) Stability of pristine surfaces and surface-H in structural relaxation and MD simulations at finite temperatures up to 1000 K. Different levels of rings represent the different stabilities, the outer the ring is, the more stable it is. The r-(110c) means the (110c) surface with surface reconstruction.It can be observed that at high temperatures, the decomposition products of surface-H include nitrogen gas and nitrogen-hydrogen compounds. Nitrogen-hydrogen compounds observed include N2H3, N3H, N3H2, N4H, N4H2, N4H3, N5H, N6H2, and N8H5. Additionally, N4H chains are observed for (110d)-H, and a small amount of H2 is also detected in (110a)-H.
Interestingly, reconstruction occurring in the pristine (110c) surface with the formation of N3 groups [Fig. 1(a)] is suppressed by H saturation. As shown in Fig. 4, after structural relaxation, the reconstruction does not occur in the H-saturated (110c). With temperature increasing to 300 K and 500 K, the reconstruction is triggered by temperature and occurs in half of (110c)-H surface, and it further extends to the whole surface at 750 K. Note that the reconstruction of (110c) surface cannot be suppressed by the CH3 saturation, and CH3 will be decomposed by the reconstruction (Fig. S5). This phenomenon makes us further convince that H saturation is a better way to stabilize the cg-N surfaces.
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Fig. Fig. 4. Structures of (110c)-H surfaces at different temperatures. (a) Structure of (110c)-H after structure relaxation. (b) Structures of (110c)-H after MD simulations at 300 K. (c) Structures of (110c)-H after MD simulations at 500 K. (d) Structures of (110c)-H after MD simulations at 750 K. Reconstruction does not occur after the structural relaxation, while half of surface has reconstruction after MD simulations at 300 K and 500 K. At 750 K, surface reconstruction is completed. To facilitate identification, reconfigured N atoms are marked with yellow circles.Based on the above discussions, we can find that although the dangling bonds are saturated in both surface-OH and surface-H, their stabilities show large difference. To understand this phenomenon, we further investigate the charger transfer between saturated groups and surfaces relying on the Bader charge analysis (Table S1 in the Supplementary Materials), and the average number of electrons transferring from saturated groups into nitrogen atoms is shown in the brackets on the y-axis tag in Fig. 2. Positive (negative) values mean electrons transfer from saturated groups to surfaces (from surfaces to saturated groups). For surface-H, surface-CH3 and surface-OH, the charge transfer is 1.39e, 1.19e, and −0.28e, respectively, and the stability of surfaces increases with the number of electrons on the surfaces (surface-OH < surface-CH3 < surface-H). The electronegativity of OH (3.49)[52] is larger than that of N (3.04),[53] and electrons would transfer from N to OH. However, the opposite process occurs when hydrogen atoms are adsorbed on the surface, because the electronegativity of H (2.20)[52] is notably smaller.
To further rationalize the charge transfer behaviors of surface-OH and surface-H, the electron density difference of (111a)-H and (111a)-OH surfaces are calculated as shown in Fig. 5, which confirms charge transfers from H to N in (111a)-H surface and N to OH in (111a)-OH surface. The results clearly show that electron transfer to nitrogen is beneficial to enhance the surface stabilities, while the opposite process leads to the decreasing stability. Therefore, although the dangling bonds are saturated in surface-OH, the OH saturation takes electrons from the surfaces and cannot promote their stabilities. However, H adsorption not only saturates the dangling bonds but also transfers electrons to the surfaces, giving rise to a very high stability of cg-N surfaces.
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Fig. Fig. 5. (a) Electron density difference (EDD) of (111a)-H surface. (b) EDD of (111a)-OH surface. The curves are plotted along the z axis of the structures, which are shown in the insets. The local integral curve shown in red presents the electron gain (positive values) and loss (negative values), and the integral curve shown in blue is the integral of the local integral curve. Isosurface in the structures is set to 0.003 e/Bohr3, and orange (blue) isosurface presents positive (negative) values of electron density difference.In summary, based on the first-principles and molecular dynamics method, stabilities of cg-N surfaces are systematically investigated, and effects of pressure, temperature, and saturations with H, OH, and CH3 on the surface stabilities are presented. For pristine cases, only the reconfigured (110c) surfaces with linear N3 groups adsorption can exist at 300 K, and other surfaces are very brittle, especially the (110b) and (110d) surfaces will collapse totally just after structural relaxation. However, the decompositions of surfaces will be suppressed at high pressure, indicating that surface instability causes the cg-N instability at low pressure. Interestingly, by H saturation, all of investigated surfaces can be stabilized not only under ambient conditions but also at 750 K, since H atoms can saturate dangling bonds combined with transferring electrons to the surfaces. OH saturation cannot improve the stabilities of surfaces, because it gets electrons from the surfaces.
We propose the following plan to realize hydrogen surface-saturated cg-N: The most part of the sample chamber of the diamond anvil cell is filled with nitrogen gas, and small part is filled with a suitable hydrogen-rich material (e.g., ammonia borane) for providing hydrogen source by heating. In the process of synthesizing cg-N, the N2-filled part is heated by laser heating, while the part filled with hydrogen-rich material remains unheated. After cg-N is synthesized, the hydrogen-rich material can be heated to generate hydrogen, which can saturate the surface of cg-N. Besides the high-pressure synthesis, our results can also provide effective guidance for future synthesis of cg-N under atmospheric pressure. For example, an acidic environment is helpful to improve the stabilities of cg-N and its relatives. Furthermore, materials, which can be more conducive to transferring electrons to neighbors, such as graphene and carbon nanotubes with a band gap as small as possible, can be used as assistant to improve the stabilities of polymeric nitrogen.
Acknowledgements: This work was supported by the National Natural Science Foundation of China (Grant No. U2030114), and CASHIPS Director’s Fund (Grant No. YZJJ202207-CX). The calculations were partly performed at Center for Computational Science of CASHIPS, the ScGrid of Supercomputing Center and Computer Network Information Center of Chinese Academy of Sciences, and the Hefei Advanced Computing Center. -
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