Modeling of the self-limited growth in catalytic chemical vapor deposition of graphene

Kim, Hokwon; Saiz, Eduardo; Chhowalla, Manishkumar; Mattevi, Cecilia

doi:10.1088/1367-2630/15/5/053012

Cited by 54 publications

(44 citation statements)

References 68 publications

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“…In addition, it is well documented in the literature that temperature, carbon precursor partial pressure, and its ratio to hydrogen can have a significant influence on the GND. 4,14,29,46−48 Our results of different pretreatment approaches summarized in Figure 1 are based on a growth temperature of 1065 °C and a growth atmosphere of 250 sccm Ar, 26 sccm H 2 , and 9 sccm CH 4 (0.1% diluted in Ar). Industrial high-throughput CVD not only requires a low GND but also reasonably high growth rates to grow continuous films.…”

Section: Resultsmentioning

confidence: 99%

Understanding and Controlling Cu-Catalyzed Graphene Nucleation: The Role of Impurities, Roughness, and Oxygen Scavenging

et al. 2016

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The mechanism by which Cu catalyst pretreatments control graphene nucleation density in scalable chemical vapor deposition (CVD) is systematically explored. The intrinsic and extrinsic carbon contamination in the Cu foil is identified by time-of-flight secondary ion mass spectrometry as a major factor influencing graphene nucleation and growth. By selectively oxidizing the backside of the Cu foil prior to graphene growth, a drastic reduction of the graphene nucleation density by 6 orders of magnitude can be obtained. This approach decouples surface roughness effects and at the same time allows us to trace the scavenging effect of oxygen on deleterious carbon impurities as it permeates through the Cu bulk. Parallels to well-known processes in Cu metallurgy are discussed. We also put into context the relative effectiveness and underlying mechanisms of the most widely used Cu pretreatments, including wet etching and electropolishing, allowing a rationalization of current literature and determination of the relevant parameter space for graphene growth. Taking into account the wider CVD growth parameter space, guidelines are discussed for high-throughput manufacturing of “electronic-quality” monolayer graphene films with domain size exceeding 1 mm, suitable for emerging industrial applications, such as electronics and photonics.

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Section: Resultsmentioning

confidence: 99%

Understanding and Controlling Cu-Catalyzed Graphene Nucleation: The Role of Impurities, Roughness, and Oxygen Scavenging

et al. 2016

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“…Three methods of graphene preparation were employed: (i) segregation of carbon from the bulk of the metal, (ii) chemical vapor deposition of hydrocarbons, and (iii) carbon vapor deposition (Xu et al 2013). Despite intensive investigations, many fundamental aspects of the graphene nucleation are still not fully understood (Mehdipour and Ostrikov 2012, Kim et al 2013.…”

Section: Carbon Depositsmentioning

confidence: 99%

On thermodynamic equilibrium of carbon deposition from gaseous C-H-O mixtures: updating for nanotubes

Jaworski

Zakrzewska

Pianko‐Oprych

2017

Reviews in Chemical Engineering

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AbstractExtensive literature information on experimental thermodynamic data and theoretical analysis for depositing carbon in various crystallographic forms is examined, and a new three-phase diagram for carbon is proposed. The published methods of quantitative description of gas-solid carbon equilibrium conditions are critically evaluated for filamentous carbon. The standard chemical potential values are accepted only for purified single-walled and multi-walled carbon nanotubes (CNT). Series of C-H-O ternary diagrams are constructed with plots of boundary lines for carbon deposition either as graphite or nanotubes. The lines are computed for nine temperature levels from 200°C to 1000°C and for the total pressure of 1 bar and 10 bar. The diagram for graphite and 1 bar fully conforms to that in (Sasaki K, Teraoka Y. Equilibria in fuel cell gases II. The C-H-O ternary diagrams. J Electrochem Soc 2003b, 150: A885–A888). Allowing for CNTs in carbon deposition leads to significant lowering of the critical carbon content in the reformates in temperatures from 500°C upward with maximum shifting up the deposition boundary O/C values by about 17% and 28%, respectively, at 1 and 10 bar.

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“…One of the approaches of growing an AB‐stacked bilayer graphene is by chemical vapor deposition (CVD) method. The CVD approach has demonstrated an excellent capability of growing wafer‐scale high‐quality AB‐stacked bilayer graphene . In CVD graphene growth, copper (Cu) is the most favorable substrate because of it has lower carbon solubility (i.e.…”

Section: Introductionmentioning

confidence: 99%

“…The lower decomposition rate of methane by Cu is advantageous for wafer‐scale monolayer graphene growth but disadvantageous for wafer‐scale bilayer graphene growth as it requires more carbon atoms. In fact, it is practically impossible to supply sufficient carbon atoms for wafer‐scale multilayer graphene growth on pure Cu surface . Generally, a bilayer graphene obtained on pure Cu foil is known to be incomplete (have smaller areas of bilayer) with a significant fraction of non‐AB stacking …”

Section: Introductionmentioning

confidence: 99%

Raman analysis of bilayer graphene film prepared on commercial Cu(0.5 at% Ni) foil

Bello

Dangbegnon

Oliphant

et al. 2015

J Raman Spectroscopy

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This study reports the Raman analysis of bilayer graphene films prepared on commercial dilute Cu(0.5 at% Ni) foils using atmospheric pressure chemical vapour deposition (AP-CVD). A bilayer graphene film obtained on Cu foil is known to have small-areas of bilayer (islands) with a significant fraction of non-Bernal stacking while that obtained on Cu/Ni is known to grow over a large-area with Bernal stacking. In the Raman optical microscope images, a wafer-scale monolayer and large-area bilayer graphene films were distinguished and confirmed with Raman spectra intensities ratios of 2D to G peaks. The large-area part of bilayer graphene film obtained was assisted by Ni surface segregation since Ni has higher methane decomposition rate and carbon solubility compared to Cu. The Raman data suggest a Bernal stacking order in the prepared bilayer graphene film. A four-point probe sheet resistance of graphene films confirmed a bilayer graphene film sheet resistance distinguished from that of monolayer graphene. A relatively higher Ni surface concentration in Cu(0.5 at% Ni) foil was confirmed with time-of-flight secondary ion mass spectrometry. The inhomogeneous distribution of Ni in a foil and the diverse crystallographic surface of a foil (confirmed with proton-induced X-ray emission (PIXE) and electron backscatter diffraction respectively), could be a reason for incomplete wafer-scale bilayer graphene film. The Ni surface segregation in dilute Cu(0.5 at% Ni) foil has a potential to impact on AP-CVD growth of large-area bilayer graphene film.

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Modeling of the self-limited growth in catalytic chemical vapor deposition of graphene

Cited by 54 publications

References 68 publications

Understanding and Controlling Cu-Catalyzed Graphene Nucleation: The Role of Impurities, Roughness, and Oxygen Scavenging

Understanding and Controlling Cu-Catalyzed Graphene Nucleation: The Role of Impurities, Roughness, and Oxygen Scavenging

On thermodynamic equilibrium of carbon deposition from gaseous C-H-O mixtures: updating for nanotubes

Raman analysis of bilayer graphene film prepared on commercial Cu(0.5 at% Ni) foil

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