Direct chemical conversion of graphene to boron- and nitrogen- and carbon-containing atomic layers

Gong, Yongji; Shi, Gang; Zhang, Zhuhua; Zhou, Wu; Jung, Jeil; Gao, Weilu; Ma, Lulu; Yang, Yang; Yang, Shubin; Ge, You; Vajtai, Róbert; Xu, Qianfan; MacDonald, Allan H.; Yakobson, Boris I.; Lou, Jun; Liu, Zheng; Ajayan, Pulickel M.

doi:10.1038/ncomms4193

Cited by 221 publications

(244 citation statements)

References 39 publications

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“…The resistance decrease when heating temperature (graphene domain) increases (Figure 6b). 9 The epitaxial, single-crystal hybridized h-BN/graphene layer on a wide-gap semiconductor substrate can facilitate device applications for the hybridized structure without a transfer process, as demonstrated for epitaxial graphene on a SiC substrate. SEM experiments.…”

Section: Resultsmentioning

confidence: 99%

Epitaxial Growth of a Single-Crystal Hybridized Boron Nitride and Graphene Layer on a Wide-Band Gap Semiconductor

et al. 2015

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Vertical and lateral heterogeneous structures of two-dimensional (2D) materials have paved the way for pioneering studies on the physics and applications of 2D materials. A hybridized hexagonal boron nitride (h-BN) and graphene lateral structure, a heterogeneous 2D structure, has been fabricated on single-crystal metals or metal foils by chemical vapor deposition (CVD).However, once fabricated on metals, the h-BN/graphene lateral structures require an additional transfer process for device applications, as reported for CVD graphene grown on metal foils. Here, we demonstrate that a single-crystal h-BN/graphene lateral structure can be epitaxially grown on a wide-gap semiconductor, SiC(0001). First, a single-crystal h-BN layer with the same orientation as bulk SiC was grown on a Si-terminated SiC substrate at 850 ℃ using borazine molecules.Second, when heated above 1150 ℃ in vacuum, the h-BN layer was partially removed and, subsequently, replaced with graphene domains. Interestingly, these graphene domains possess the same orientation as the h-BN layer, resulting in a single-crystal h-BN/graphene lateral structure on a whole sample area. For temperatures above 1600 ℃ , the single-crystal h-BN layer was completely replaced by the single-crystal graphene layer. The crystalline structure, electronic band structure, and atomic structure of the h-BN/graphene lateral structure were studied by using low energy electron diffraction, angle-resolved photoemission spectroscopy, and scanning tunneling microscopy, respectively. The h-BN/graphene lateral structure fabricated on a wide-gap semiconductor substrate can be directly applied to devices without a further transfer process, as reported for epitaxial graphene on a SiC substrate.

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Section: Resultsmentioning

confidence: 99%

Epitaxial Growth of a Single-Crystal Hybridized Boron Nitride and Graphene Layer on a Wide-Band Gap Semiconductor

et al. 2015

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“…Raman signal for the h-BCN sample is not observed (Fig. S3), due to the structural distortion induced by the C substitution in layered h-BN, instead of a phase-separated structure made of C domains and BN [28]. This however indicates the doping of carbon in the h-BN crystal narrows the band gap by substitution of B with C, by which the hybridization of B 2p with C 2p orbitals also widens the density states of the conduction band that facilitates electron migration, being promising for photoredox catalysis.…”

Section: Resultsmentioning

confidence: 99%

“…An interesting case of such a layered material is ternary h-BCN with tuneable ba nd gap energies between graphene (zero bandgap) and h-BN (bandgap = 5.6 eV) [27], which have the same atomic structure and share many similar properties. The hybridized phases of the two two-dimensional (2D) materials by atomic mixture of B, N, and C with broad composition ranges to create various layered semiconducting structures would produce new material functions complementary to graphene and h-BN, enabling a wide variety of electronic structures, applications and properties [28][29][30]. Such an emerging family of chemically inert and mechanically strong 2D materials practically allows the bandgap-engineered applications in heterogeneous photocatalysis by creating a medium-gap ternary semiconductor, in which the band gap, redox energy levels, p/n-type properties and surface acid-base chemistry can in principle be modulated by rational design and synthesis [31,32].…”

mentioning

confidence: 99%

Photocatalytic water oxidation by layered Co/h-BCN hybrids

et al. 2015

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The search for new materials has progressed from metal-based photocatalysts to elemental semiconductors (C, Si, P, S, B) [11][12][13][14][15] and recently to metal-free binary materials and polymers, such as carbon nitride [16], boron carbide [17] and conjugated semiconductors [18][19][20]. These researches indicate that photon absorbing materials can be constituted by using lightweight elements such as carbon, nitrogen, and boron, opening up new opportunities for the selection of innovative and intriguing materials for artificial photosynthesis. It is of particular interest that some of these elements themselves (graphene [21], silicone [22]) or their combinations (h-BN, g-C 3 N 4 ) [23] can form layered structures with reduced thickness comparable to charge-diffusion distance, and thus if a semiconducting electronic structure was imparted in these materials, the fast separation of light-induced charge carrier would significantly benefit surface photoredox process that relied on the excitation and separation of electron-hole pairs and their subsequent participation in surface chemical reactions [24][25][26]. An interesting case of such a layered material is ternary h-BCN with tuneable ba nd gap energies between graphene (zero bandgap) and h-BN (bandgap = 5.6 eV) [27], which have the same atomic structure and share many similar properties. The hybridized phases of the two two-dimensional (2D) materials by atomic mixture of B, N, and C with broad composition ranges to create various layered semiconducting structures would produce new material functions complementary to graphene and h-BN, enabling a wide variety of electronic structures, applications and properties [28][29][30]. Such an emerging family of chemically inert and mechanically strong 2D materials practically allows the bandgap-engineered applications in heterogeneous photocatalysis by creating a medium-gap ternary semiconductor, in which the band gap, redox energy levels, p/n-type properties and surface acid-base chemistry can in principle be modulated by rational design and synthesis [31,32].A hexagonal boron carbon nitride (h-BCN) semiconductor was applied to intercalate cobalt ions to catalyze oxygen evolution reaction (OER) with light illumination, without using noble metals. The h-BCN with high specific surface area showed a strong chemical affinity towards metal ions due to the "lop-sided" densities characteristic of ionic B-N bonding, enabling the creation of metal/h-BCN hybrid layered structures with unique properties. As exemplified here by Co/h-BCN for water oxidation catalysis, after intercalating cobalt ions in the h-BCN host, the photocatalytic activity of the resultant layered hybrid is optimized due to their synergic catalysis that promotes charge separation and lowers reaction barriers. This finding promises a new nobel-metal-free nanocompsite using cost-acceptable and earth-abundant sust ances for photocatalytic OER, and enables the facile design of duel catalytic cascades by merging transition metal catalysis with h-BCN (photo)catalys...

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“…2 The atomic layered structure of hBN is also well suited as a substrate for transferable 2 and flexible device applications. Moreover, the ability of hBN to form alloy 13 or lateral heterostructures 14 with graphene is noteworthy for fabricating sophisticated on-demand devices. The recent progress of large-scale hBN synthesis with precisely controlled thickness via chemical vapor deposition techniques 11 may allow the integration of semiconductors with wafers based on conventional microfabrication processes.…”

Section: Introductionmentioning

confidence: 99%

Architectured van der Waals epitaxy of ZnO nanostructures on hexagonal BN

Hong

Kim

et al. 2014

NPG Asia Mater

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Heteroepitaxy of semiconductors on two-dimensional (2-d) atomic layered materials enables the use of flexible and transferable inorganic electronic and optoelectronic devices in various applications. Herein, we report the shape-and morphology-controlled van der Waals (vdW) epitaxy of ZnO nanostructures on hexagonal boron nitride (hBN) insulating layers for an architectured semiconductor integration on the 2-d layered materials. The vdW surface feature of the 2-d nanomaterials, because of the surface free of dangling bonds, typically results in low-density random nucleation-growth in the vdW epitaxy. The difficulty in controlling the nucleation sites was resolved by artificially formed atomic ledges prepared on hBN substrates, which promoted the preferential vdW nucleation-growth of ZnO specifically along the designed ledges. Electron microscopy revealed crystallographically domain-aligned incommensurate vdW heteroepitaxial relationships, even though ZnO/hBN is highly latticemismatched. First-principles theoretical calculations confirmed the weakly bound, noncovalent binding feature of the ZnO/hBN heterostructure. Electrical characterizations of the ZnO nanowall networks grown on hBN revealed the excellent electrical insulation properties of hBN substrates. An ultraviolet photoconductor device using the vdW epitaxial ZnO nanowall networks/ hBN heterostructure was further demonstrated as an example of hBN substrate-based device applications. The architectured heteroepitaxy of semiconductors on hBN is thus expected to create many other device arrays that can be integrated on a piece of substrate with good electrical insulation for use in individual device operation.

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Direct chemical conversion of graphene to boron- and nitrogen- and carbon-containing atomic layers

Cited by 221 publications

References 39 publications

Epitaxial Growth of a Single-Crystal Hybridized Boron Nitride and Graphene Layer on a Wide-Band Gap Semiconductor

Epitaxial Growth of a Single-Crystal Hybridized Boron Nitride and Graphene Layer on a Wide-Band Gap Semiconductor

Photocatalytic water oxidation by layered Co/h-BCN hybrids

Architectured van der Waals epitaxy of ZnO nanostructures on hexagonal BN

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