Chemical bonding, structure, and hardness of carbon nitride thin films

Zheng, Weitao; Yu, Weili; Li, H.B.; Wang, Y.M.; Cao, Peijiang; Jin, Zengsun; Broitman, Esteban; Sundgren, J.‐E.

doi:10.1016/s0925-9635(00)00314-9

Cited by 15 publications

(10 citation statements)

References 11 publications

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“…Carbon nitride materials have attracted continuous attention in research over past decades as indicated by extensive efforts from both theory , and experiments. − Sustained interest in nitrogen-bearing, carbon-rich materials stems from their multiple functionalities and diverse applications. − For example, cubic carbon nitride ( c -C 3 N 4 ) is predicted to have hardness comparable to diamond, , whereas graphitic carbon nitride ( g -C 3 N 4 ) has been demonstrated to act as a photocatalyst for various redox reactions. − Furthermore, nitrogen-doped carbon materials often exhibit excellent properties as compared with their pure carbon counterparts, e.g., conductivity, basicity, oxidation stability, and catalytic activity, although these properties are highly dependent on the amount of nitrogen incorporated within the structure. − When long-range order within carbon nitride materials is lacking, disordered structures containing sp 2 and sp 3 bonding may still exhibit outstanding mechanical properties, − which is fundamentally important for the realization of three-dimensional, crystalline carbon nitride solids.…”

Section: Introductionmentioning

confidence: 99%

From Linear Molecular Chains to Extended Polycyclic Networks: Polymerization of Dicyanoacetylene

et al. 2017

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Dicyanoacetylene (C4N2) is an unusual energetic molecule with alternating triple and single bonds (think miniature, nitrogen-capped carbyne), which represents an interesting starting point for the transformation into extended carbon–nitrogen solids. While pressure-induced polymerization has been documented for a wide variety of related molecular solids, precise mechanistic details of reaction pathways are often poorly understood and the characterization of recovered products is typically incomplete. Here, we study the high-pressure behavior of C4N2 and demonstrate polymerization into a disordered carbon–nitrogen network that is recoverable to ambient conditions. The reaction proceeds via activation of linear molecules into buckled molecular chains, which spontaneously assemble into a polycyclic network that lacks long-range order. The recovered product was characterized using a variety of optical spectroscopies, X-ray methods, and theoretical simulations and is described as a predominately sp2 network comprising “pyrrolic” and “pyridinic” rings with an overall tendency toward a two-dimensional structure. This understanding offers valuable mechanistic insights into design guidelines for next-generation carbon nitride materials with unique structures and compositions.

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Section: Introductionmentioning

confidence: 99%

From Linear Molecular Chains to Extended Polycyclic Networks: Polymerization of Dicyanoacetylene

et al. 2017

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“…In particular, x-ray photoelectron spectroscopy ͑XPS͒ 1,2,4 -6 and vibrational spectroscopy [7][8][9][10][11] measurements have been the most common techniques used to investigate this subject. However, interpretation of these data varies widely in the literature.…”

Section: Introductionmentioning

confidence: 99%

Bonding in hard and elastic amorphous carbon nitride films investigated using15N,13C

et al. 2003

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The nitrogen bonding in hard and elastic amorphous carbon nitride (a-CN x ) films is examined with 15 N, 13 C, and 1 H nuclear magnetic resonance ͑NMR͒ spectroscopy. Films were deposited by dc magnetron sputtering, in a pure nitrogen discharge on Si͑001͒ substrates at 300°C. Nanoindentation tests revealed an elastic recovery of 80%, a hardness of 5 GPa, and an elastic modulus of 47 GPa. The NMR results show that nitrogen bonding in this material is consistent with sp 2 hybridized nitrogen incorporated in an aromatic carbon environment. The data also indicate that the a-CN x prepared for this study has very low hydrogen content and is hydrophilic. Specifically, analysis of 15 N and 13 C cross polarization magic angle spinning and 1 H NMR experiments suggests that water preferentially protonates nitrogen sites.

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“…[1][2][3][4] The most widely accepted model that correlates the structure of hard and elastic a-CN x with its mechanical properties proposes that the material consists of buckled graphitic segments with incorporated nitrogen, and that these segments are crosslinked by sp 3 bonded carbon. 1,2,5,6 Electron energy loss spectroscopy 2,7,8 ͑EELS͒ and near-edge x-ray absorption fine-structure spectroscopy 3,9 ͑NEXAFS͒ have been used to try to examine the relative fractions of sp 2 and sp 3 hybridized carbon bonded to carbon in a-CN x . However to date, no reliable quantitative measurements of the amount of sp 3 hybridized carbon has been reported in the literature.…”

Section: Introductionmentioning

confidence: 99%

Hard and elastic amorphous carbon nitride thin films studied by13Cnuclear magnetic resonance spectroscopy

Gammon

Malyarenko

Kraft³

et al. 2002

Phys. Rev. B

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The chemical bonding of hard and elastic amorphous carbon nitride (a-CN x) thin films was examined using solid-state 13 C NMR spectroscopy. The films were deposited by DC magnetron sputtering in a pure nitrogen discharge on Si͑001͒ substrates at 300°C. Nanoindentation tests reveal a recovery of 80%, a hardness of 5 GPa, and an elastic modulus of 47 GPa. This combination of low modulus and high strength means the material can be regarded as hard and elastic; the material gives when pressed on and recovers its shape when the load is released. The 13 C NMR results conclusively demonstrate that hard and elastic a-CN x has an sp 2 carbon bonded structure and that sp 3 hybridized carbons are absent. Our results stand in contrast with earlier work that proposed that the interesting mechanical properties of hard and elastic a-CN x were due, in part, to sp 3 bonded carbon.

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Chemical bonding, structure, and hardness of carbon nitride thin films

Cited by 15 publications

References 11 publications

From Linear Molecular Chains to Extended Polycyclic Networks: Polymerization of Dicyanoacetylene

From Linear Molecular Chains to Extended Polycyclic Networks: Polymerization of Dicyanoacetylene

Bonding in hard and elastic amorphous carbon nitride films investigated using15N,13C

Hard and elastic amorphous carbon nitride thin films studied by13Cnuclear magnetic resonance spectroscopy

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