Chemical Vapor Deposition Growth Of Graphene Research Articles

Silicon oxide particles size evolution during CVD graphene growth on Cu substrates

Chemical vapor deposition (CVD) on metal substrates is presently the remarkably route for the synthesis of high-quality continuous graphene films at a large scale. Whereas, during the thermal processing procedure in the quartz tube, the formation of silicon oxide particles would degrade the performance of graphene. To better understand the origin of these particles , a series of CVD graphene growth experiments with were conducted on the Cu substrates. In this paper, we investigated the main component and morphology of the particles by X-Ray photoelectron spectroscopy (XPS), energy dispersive spectrometry (EDS) measurement in scanning electron microscopy (SEM) and revealed that the silicon oxide particles gradually increased in diameter across the graphene films on the Cu surface, which was found to be correlated with the working time of the quartz products. Raman spectroscopy was also applied to prove the drawback consequence of the contamination on the quality of the CVD graphene film. To mitigate this issue, we further propose a modification of the CVD system that a coaxial alumina or BN tube inside the quartz tube to screen the contaminants bringing about improved graphene growth.

A Wrinkling and Etching-Assisted Regrowth Strategy for Large-Area Bilayer Graphene Preparation on Cu.

Bilayer graphene is a contender of interest for functional electronic applications because of its variable band gap due to interlayer interactions. Graphene growth on Cu is self-limiting, thus despite the fact that chemical vapor deposition (CVD) has made substantial strides in the production of monolayer and single-crystal graphene on Cu substrates, the direct synthesizing of high-quality, large-area bilayer graphene remains an enormous challenge. In order to tackle this issue, we present a simple technique using typical CVD graphene growth followed by a repetitive wrinkling-etching-regrowth procedure. The key element of our approach is the rapid cooling process that causes high-density wrinkles to form in the monolayer area rather than the bilayer area. Next, wrinkled sites are selectively etched with hydrogen, exposing a significant portion of the active Cu surface, and leaving the remaining bilayer areas, which enhance the nucleation and growth of the second graphene layer. A fully covered graphene with 78 ± 2.8% bilayer coverage and a bilayer transmittance of 95.6% at room temperature can be achieved by modifying the process settings. Bilayer graphene samples are examined using optical microscopy (OM), scanning electron microscopy (SEM), Raman spectroscopy, and an atomic force microscope (AFM) during this process. The outcomes of our research are beneficial in clarifying the growth processes and future commercial applications of bilayer graphene.

Numerical Simulation of a Simplified Reaction Model for the Growth of Graphene via Chemical Vapor Deposition in Vertical Rotating Disk Reactor

The process of graphene growth by CVD involves a series of complex gas-phase surface chemical reactions, which generally go through three processes, including gas phase decomposition, surface chemical reaction, and gas phase diffusion. The complexity of the CVD process for growing graphene is that it involves not only chemical reactions but also mass, momentum, and energy transfer. To solve these problems, the method of numerical simulation combined with the reactor structure optimization model provides a good tool for industrial production and theoretical research to explore the influencing factors of the CVD growth of graphene. The objective of this study was to establish a simplified reaction model for the growth of graphene by chemical vapor deposition(CVD) in a vertical rotating disk reactor (VRD). From a macroscopic modeling perspective, computational fluid dynamics (CFD) was used to investigate the conditions for the growth of graphene by chemical vapor deposition in a high-speed rotating vertical disk reactor on a copper substrate surface at atmospheric pressure (101,325 Pa). The effects of gas temperature, air inlet velocity, base rotation speed, and material ratio on the surface deposition rate of graphene in a VRD reactor were studied, and the technological conditions for the preparation of graphene via the CVD method in a VRD reactor based on a special structure were explored. Compared with existing models, the numerical results showed the following: the ideal growth conditions of graphene prepared using a CVD method in a VRD reactor involve a growth temperature of 1310 K, an intake speed of 470 mL/min, a base speed of 300 rpm, and an H2 flow rate of 75 sccm; thus, more uniform graphene with a better surface density and higher quality can be obtained. The effect of the carbon surface deposition rate on the growth behavior of graphene was studied using molecular dynamics (MD) from a microscopic perspective. The simulation showed that the graphene surface deposition rate could control the nucleation density of graphene. The combination of macro- and microsimulation methods was used to provide a theoretical reference for the production of graphene.

Multiscale Model of CVD Growth of Graphene on Cu(111) Surface.

Due to its outstanding properties, graphene has emerged as one of the most promising 2D materials in a large variety of research fields. Among the available fabrication protocols, chemical vapor deposition (CVD) enables the production of high quality single-layered large area graphene. To better understand the kinetics of CVD graphene growth, multiscale modeling approaches are sought after. Although a variety of models have been developed to study the growth mechanism, prior studies are either limited to very small systems, are forced to simplify the model to eliminate the fast process, or they simplify reactions. While it is possible to rationalize these approximations, it is important to note that they have non-trivial consequences on the overall growth of graphene. Therefore, a comprehensive understanding of the kinetics of graphene growth in CVD remains a challenge. Here, we introduce a kinetic Monte Carlo protocol that permits, for the first time, the representation of relevant reactions on the atomic scale, without additional approximations, while still reaching very long time and length scales of the simulation of graphene growth. The quantum-mechanics-based multiscale model, which links kinetic Monte Carlo growth processes with the rates of occurring chemical reactions, calculated from first principles makes it possible to investigate the contributions of the most important species in graphene growth. It permits the proper investigation of the role of carbon and its dimer in the growth process, thus indicating the carbon dimer to be the dominant species. The consideration of hydrogenation and dehydrogenation reactions enables us to correlate the quality of the material grown within the CVD control parameters and to demonstrate an important role of these reactions in the quality of the grown graphene in terms of its surface roughness, hydrogenation sites, and vacancy defects. The model developed is capable of providing additional insights to control the graphene growth mechanism on Cu(111), which may guide further experimental and theoretical developments.

Direct CVD Growth of Transferable 3D Graphene for Sensitive and Flexible SERS Sensor

Three-dimensional (3D) graphene (Gr) has been successfully grown on a patterned sapphire substrate (PSS) with very low mismatch between Gr and the sapphire nanostructure through metal-catalyst-assisted chemical vapor deposition (CVD). However, the transfer of the 3D Gr film without compromising the structural integrity of Gr is challenging because of the low etching rate of PSS. For easy and high-quality transfer of 3D Gr, we propose to coat a transfer-support layer (TSL) on PSS before direct CVD growth of 3D Gr. The TSL is directly deposited on PSS by atomic layer deposition without causing any structural changes in the substrate, as verified through atomic force microscopy (AFM). Few-layer 3D Gr is conformally produced along the surface of the TSL/PSS and successfully transferred onto a flexible substrate through wet-etching transfer, as confirmed by scanning electron microscopy, AFM, and Raman spectroscopy studies. We also present the fabrication of a sensitive and flexible surface-enhanced Raman scattering sensor based on 3D Gr on PMMA with high detection performance for low concentrations of R6G (10-9 M). The proposed transfer method with TSL is expected to broaden the use of 3D graphene in next-generation device applications.

Increasing coverage of mono-layer graphene grown on hexagonal boron nitride

Graphene sitting on hexagonal boron nitride (h-BN) always exhibits excellent electrical properties. And the properties of graphene on h-BN are often dominated by its domain size and boundaries. Chemical vapor deposition (CVD) is a promising approach to achieve large size graphene crystal. However, the CVD growth of graphene on h-BN still faces challenges in increasing coverage of monolayer graphene because of a weak control on nucleation and vertical growth. Here, an auxiliary source strategy is adapted to increase the nucleation density of graphene on h-BN and synthesis continuous graphene films. It is found that both silicon carbide and organic polymer e.g. methyl methacrylate can assist the nucleation of graphene, and then increases the coverage of graphene on h-BN. By optimizing the growth temperature, vertical accumulation of graphitic materials can be greatly suppressed. This work provides an effective approach for preparing continuous graphene film on h-BN, and may bring a new sight for the growth of high quality graphene.

Anti-dewetting of Cu thin film on nanostructured black Si template for continuous CVD growth of monolayer graphene

The growth of high-quality continuous film of graphene on less than [Formula: see text]m-thick Cu film is proven to be a challenging task due to the solid-state dewetting of Cu during the high-temperature chemical vapor deposition (CVD) process. In this paper, we introduce the use of nanostructured black Si (b-Si) as a template for Cu evaporation to mitigate the dewetting of Cu thin film. Using a cold-wall CVD system at a process temperature of 825[Formula: see text]C, even Cu thickness, [Formula: see text] nm on polished SiO2/Si substrate is poor for maintaining Cu as a continuous film. If the polished SiO2/Si is replaced with SiO2/b-Si, the minimum [Formula: see text] nm is sufficient. According to the Cu trapping mechanism, moving Cu particle is trapped in the nanostructured trenches of SiO2/b-Si during annealing and CVD growth processes. Continuous monolayer graphene with a grain size of [Formula: see text]m without defect is obtained on Cu/SiO2/b-Si substrate. The improved adhesion of Cu to the SiO2/b-Si enables dry-transfer of graphene by mechanical peeling using a polyvinyl alcohol (PVA) film. Our solution is promising for obtaining flat graphene and a recyclable Cu/SiO2/b-Si substrate.

Complementary Chemical Vapor Deposition Fabrication for Large‐Area Uniform Graphene Glass Fiber Fabric

The lightweight, flexible, high-performance electrothermal material is in high demand in object thermal management. Graphene glass fiber fabric (GGFF) is characterized by excellent electrical conductivity, light weight, and high flexibility, showing superiorities as an electrothermal material. However, the traditional single-carbon-precursor chemical vapor deposition (CVD) graphene growth strategy commonly suffers from the severe thickness nonuniformity of the large-sized graphene film along the gas-flowing direction. Herein, a complementary CVD graphene growth strategy based on the simultaneous introduction of high- and low-decomposition-energy-barrier mixed carbon precursors is developed. In this way, the large-area uniform GGFF with a dramatically decreased nonuniformity coefficient is fabricated (0.260 in 40cm × 4cm). GGFF-based heater presents a widely tunable temperature range (20-170°C) at low working voltage (<10V) and uniform large-area heating temperature (171.4± 3.6°C in 20cm × 15cm), which realizes remarkable anti/deicing performances under the low energy consumption (fast ice melting rate of 79s mm-1 under a low energy consumption of 0.066kWh mm-1 m-2 ). The large-area uniform GGFF possesses substantial advantages for applications in thermal management, and the complementary CVD fabrication strategy shows reliable scalability and universality, which can be extended to the synthesis of various materials.

Achievements and Challenges of Graphene Chemical Vapor Deposition Growth

AbstractGraphene, since the first successful exfoliation of graphite, has continuously attracted attention due to its remarkable properties and applications. Recently, the research focus on graphene synthesis has been directed to the controllable synthesis of large‐area and high‐quality graphene. In the last decade, there has been great progress in the chemical vapor deposition (CVD) growth of graphene. Theoretical investigations have led to an enhanced understanding of puzzles on hydrocarbon species stability, key reaction pathways, the role of hydrogen gas, the morphology of graphene islands, and the alignment of graphene on substrates. Experimentally, high‐quality graphene is epitaxially grown on both insulating and metal substrates. Progress has also been reported on low‐temperature graphene growth and on controlling the thickness and stacking of graphene layers. In this review, the authors summarize the previous theoretical and experimental studies on graphene CVD growth and discuss the future challenges on the growth of graphene i) on insulating substrates, ii) at low temperature, iii) with controllable thickness, and iv) with selected stacking twist angles. The authors assert that the key to the continuous advancement of graphene growth is the synergy of experimental and theoretical investigations.

Spiral Growth of Adlayer Graphene.

The morphology of as-grown graphene in chemical vapor deposition (CVD) experiments is sensitive to the reaction environment. Understanding the mechanism of formation of different graphene morphologies is essential to achieve controlled graphene CVD growth. Here the growth and formation mechanism of adlayer graphene spirals are reported. An adlayer graphene spiral is formed by fast propagation of the tips of spiral arms along the edge of the first graphene layer. The driving force to form spirals is the limited availability of carbon diffusing from the Cu surface through the edge of the first graphene layer. In addition, it is found that graphene onions are formed by overlapping graphene spirals with clockwise and anticlockwise arms. Based on these features, a kinetic Monte Carlo (kMC) method is demonstrated using which all the observed graphene spiral structures are successfully reproduced at the atomic level. This study thus unravels the hither-to unresolved mechanism of graphene onion growth and paves the way to the controllable growth of few-layer graphene by increasing the carbon supply at the edge of the first layer graphene.

Synergistic Effect of Cu2 O Mesh Pattern on High-Facet Cu Surface for Selective CO2 Electroreduction to Ethanol.

Although the electroconversion of carbon dioxide (CO2 ) into ethanol is considered to be one of the most promising ways of using CO2 , the ethanol selectivity is less than 50% because of difficulties in designing an optimal catalyst that arise from the complicated pathways for the electroreduction of CO2 to ethanol. Several approaches including the fabrication of oxide-derived structures, atomic surface control, and the Cu+ /Cu interfaces have been primarily used to produce ethanol from CO2 . Here, a combined structure with Cu+ and high-facets as electrocatalysts is constructed by creating high-facets of wrinkled Cu surrounded by Cu2 O mesh patterns. Using chemical vapor deposition graphene growth procedures, the insufficiently grown graphene is used as an oxidation-masking material, and the high-facet wrinkled Cu is simultaneously generated during the graphene growth synthesis. The resulting electrocatalyst shows an ethanol selectivity of 43% at -0.8V versus reversible hydrogen electrode, which is one of the highest ethanol selectivity values reported thus far. This is attributed to the role of Cu+ in enhancing CO binding strength, and the high-facets, which favor C-C coupling and the ethanol pathway. This method for generating the combined structure can be widely applicable not only for electrochemical catalysts but also in various fields.

Surface Engineering of Substrates for Chemical Vapor Deposition Growth of Graphene and Applications in Electronic and Spintronic Devices

Controllable synthesis of large-scale and high-quality graphene film is a basis for development of electronic and spintronic devices. Chemical vapor deposition (CVD) has been considered as a potential method for the industrialized preparation of high-quality graphene. The substrate in CVD is used to support graphene and even help graphene grow. Different substrates may lead to different graphene growth results. Therefore, it is of great importance to select appropriate substrates and growth strategies. In addition, the performance demands of advanced device also urgently require high-quality CVD-derived graphene supports. In this review, we summarize the current advances in surface engineering on substrates for CVD growth of graphene. Surface engineering involves anisotropic disordered, anisotropic ordered, and isotropic homogeneous surfaces of catalytic substrates, and surfaces of insulating substrates. Meanwhile, we describe how to use different surface engineering techniques to control the orientation of graphene domains, grow large-area single-crystal graphene domains, and regulate graphene layers. This information will provide a reference for the effective selection of substrates. Moreover, we review the current progress of graphene in the fields of charge and spin transport, demonstrating that graphene has broad prospects in the next generation of communications and storage. Finally, the opportunities and challenges in the controllable CVD-derived preparation of graphene and its application are discussed.

Toward large-scale CVD graphene growth by enhancing reaction kinetics via an efficient interdiffusion mediator and mechanism study utilizing CFD simulations

BackgroundThe yield rate for the synthesis of large-area and high-quality graphene, based on the chemical vapor deposition (CVD) method, is limited by the reactor size of a tubular furnace. Additionally, the reported methods to achieve a high-throughput process are still challenging. Currently, the rolled-up or vertically stacked configuration setup is applied to increase the loading growth. However, the reported methods limit the kinetic reaction of CVD growth and lead to the degradation of the uniformity and crystallinity of as-grown graphene. MethodsHere, we propose a novel method to produce a high-yield and uniform monolayer graphene film by helical stacking of Cu with highly porous carbon cloth as an efficient interdiffusion mediator. Additionally, computational fluid dynamics (CFD) is applied to simulate the dynamic distribution within the mediator. Significant FindingsThis method allows the rapid synthesis of graphene films of up to 900 cm2 for each batch of growth in a 1-inch furnace. Graphene with optimized conditions exhibits a high crystallinity (ID/IG: 0.16) and electrical conductivity (760 Ω/sq). The comprehensive study on recipe optimization together with the multiphysical simulation suggests that the proposed carbon cloth is an ideal spacing mediator for CVD graphene with a high Cu-loading density. This enhancement is attributed to the homogeneous interdiffusion of reactive gas/species in both the transverse and radial directions, resulting in homogeneous nucleation and equivalent kinetic growth. The capacity could reach 15.56 m2/hour in an 8-inch system. The CFD simulation indicates that the porous mediator can improve gas distribution and balance the pressure between the Cu foils to enhance high-yield graphene synthesis. This method provides an efficient strategy for the synthesis of high-throughput and large-area CVD graphene films, which is beneficial for cost-effective and versatile graphene-based applications.

Chemical Vapor Deposition of Graphene on Cu-Ni Alloys: The Impact of Carbon Solubility

Chemical vapour deposition (CVD) is the most promising graphene synthesis route for film and electronic applications but the growth mechanism is still not fully understood. Herein, we investigate the role of the solubility of carbon in the underlying growth substrate on the CVD growth of graphene. A range of Cu-Ni alloys compositions that cover the carbon (C) solubility range between low C solubility (pure Cu) and high C solubility (pure Ni) were used as the catalytic growth substrates. The CVD of graphene on Cu-Ni alloys showed a transition from bilayer graphene (BLG) to few-layer graphene (FLG) at a substrate Ni concentration of 45 wt.%, which was attributed to an increase in the bulk diffusion of C. The Cu-rich alloys had a high graphene coverage (BLG) at a fast-cooling rate (367 °C/min), while the Ni-rich alloys had a low coverage (FLG) under the same cooling condition. In contrast, at slow cooling rates (27 °C/min), the Cu-rich alloys had a low coverage of graphene (BLG) and the Ni-rich alloys had a high coverage of graphene (FLG). Glow discharge optical emission spectroscopy (GDOES) was used to profile the subsurface composition, particularly the C concentration, as a function of depth.

Chemical Vapor Deposition of N-Doped Graphene through Pre-Implantation of Nitrogen Ions for Long-Term Protection of Copper.

Nitrogen-doped graphene (NG) was synthesized through the chemical vapor deposition (CVD) of graphene on Cu substrates, which were pre-implanted with N ions by the ion implantation method. The pre-implanted N ions in the Cu substrate could dope graphene by the substitution of C atoms during the CVD growth of graphene, forming NG. Based on this, NG’s long-term protection properties for Cu were evaluated by ambient exposure for a corrosion test. The results showed that NG can obviously reduce the natural oxidation of Cu in the long-term exposure compared with the case of pristine graphene (PG) coated on Cu. Moreover, with the increase in pre-implanted N dose, the formed NG’s long-term protection for Cu improved. This indicates that the modification of graphene by N doping is an effective way to improve the corrosion resistance of the PG coating owing to the reduction in its conductivity, which would inhibit galvanic corrosion by cutting off electron transport across the interface in their long-term protection. These findings provide insight into corrosion mechanisms of the graphene coating and correlate with its conductive nature based on heteroatoms doping, which is a potential route for improving the corrosion resistance of graphene as an effective barrier coating for metals.

Recent Progress on CVD Growth of Graphene from a Liquid Carbon Precursor

Graphene has become a remarkable highlight of advanced material research because of its far superior properties compared to other materials. Chemical vapor deposition (CVD) has emerged as an essential method for scalable production and large area graphene for various applications. Various carbon precursors have been reported for graphene production as they can dramatically impact the graphene growth yield. In the early years of graphene CVD growth, hydrocarbon gases such as methane and acetylene have become favorable carbon precursors because of their stability at elevated temperature and controllable growth. However, hydrocarbon gases are known as explosives and toxic, therefore require a growth system with a high degree of safety and handling precautions. With the limitations mentioned above, liquid carbon source may change the graphene growth landscape as it is relatively inexpensive, non-explosive compared to the conventional gaseous precursor. This article aims to review a detailed synthesis of large-area graphene using liquid carbon precursors via the CVD technique. Challenges and future perspectives are highlights.

Theoretical calculation boosting the chemical vapor deposition growth of graphene film

Chemical vapor deposition (CVD) is a promising method for the mass production of high-quality graphene films, and great progress has been made over the last decade. Currently, the CVD growth of graphene is being pushed to achieve further advancements, such as super-clean, ultra-flat, and defect-free materials, as well as controlling the layer, stacking order, and doping level during large-scale preparation. The production of high-quality graphene by CVD relies on an in-depth knowledge of the growth mechanisms, in which theoretical calculations play a crucial role in providing valuable insights into the energy-, time-, and scale-dependent processes occurring during high-temperature growth. Here, we focus on the theoretical calculations and discuss the recent progress and challenges that need to be overcome to achieve controllable growth of high-quality graphene films on transition-metal substrates. Furthermore, we present some state-of-the-art graphene-related structures with novel properties, which are expected to enable new applications of graphene-based materials.

High Facets on Nanowrinkled Cu via Chemical Vapor Deposition Graphene Growth for Efficient CO2 Reduction into Ethanol

Achieving high electrochemical conversion of carbon dioxide (CO2) into valuable fuels and chemicals is one of the most promising directions to address environmental and energy challenges. Although several single-crystal based studies and simulation results have reported that rich in steps on Cu (100) surfaces are favorable to convert toward C2 alcohol products, most studies are still stuck in low-index (100) facets or surface defect-derived low density of step-sites. In the present work, we report the high production of ethanol by synthesizing a wrinkled Cu catalyst with high facets via a chemical vapor deposition (CVD) graphene growth process. Under our approach, we used graphene as a guiding material to produce wrinkled Cu film for use as an electrocatalyst. The graphene-grown Cu films are not only mass-producible but composed of a high density of step-sites with high-facet atomic arrangements, including the (200) and (310) facets, which are difficult to synthesize using existing methods. The wrinkled Cu film with a unique atomic arrangement showed high ethanol selectivity, achieving 40% faradaic efficiency (FE) at −0.9 V vs reversible hydrogen electrode (RHE), one of the largest selectivity values reported thus far for a Cu-based CO2 conversion catalyst. The C2 selectivity and productivity was 57% FE and −2.2 mA/cm2 at −1.1 V vs RHE, respectively. Density functional theory (DFT) calculation results demonstrated that such a high ethanol productivity is mainly attributable to the (310) facet of the wrinkles, which feature a low C–C coupling barrier (0.5 eV) and a preferred reaction path toward ethanol among other products.

In situ kinetic studies of CVD graphene growth by reflection spectroscopy

• In situ metrology system for graphene growth based on reflectance spectroscopy. • Evolution of a microkinetic model for microscopic understanding of growth process. • Investigation of hydrogen role during graphene growth. Controllable large-scale synthesis of two-dimensional materials (2DMs) such as graphene is a prerequisite for industrial applications. Chemical vapor deposition (CVD) is currently the most widespread synthesis method as it is efficient and easy to automatize. The process itself is quite complex and poorly understood, but it is generally believed to involve a number of distinct steps such as hydrocarbon decomposition into surface-bound intermediates, diffusion on the catalytic substrate, generation of nucleation points and, finally, graphene growth. In situ monitoring and tailoring of such a complex procedure is beneficial for understanding the growth kinetics and, eventually, for controlling the graphene growth. Herein, we report on a novel metrology system based on in situ reflectance spectroscopy that has been developed for real-time monitoring of surface changes during graphene growth on Cu foils at high operating temperatures. The implementation of this technique for extracting kinetic parameters of the growth process is presented. Furthermore, a microkinetic model of graphene growth based on density-functional theory (DFT) and the hindered translator / rotator model for enthalpy and entropy corrections is constructed and used to obtain a microscopic understanding of the apparent activation energy and related rate-determining steps in graphene growth.

The Mechanism of Graphene Vapor-Solid Growth on Insulating Substrates.

Wafer-scale single-crystal graphene film directly grown on insulating substrates via the chemical vapor deposition (CVD) method is desired for building high-performance graphene-based devices. In comparison with the well-studied mechanism of graphene growth on transition metal substrates, the lack of understanding on the mechanism of graphene growth on insulating surfaces greatly hinders the progress. Here, by using first-principles calculation, we systematically explored the absorption of various carbon species CHx (x = 0, 1, 2, 3, 4) on three typical insulating substrates [h-BN, sapphire, and quartz] and reveal that graphene growth on an insulating surface is dominated by the reaction of active carbon species with the hydrogen-passivated graphene edges and thus is less sensitive to the type of the substrate. The dominating gas phase precursor, CH3, plays two key roles in graphene CVD growth on an insulating substrate: (i) to feed the graphene growth and (ii) to remove excessive hydrogen atoms from the edge of graphene. The threshold reaction barriers for the growth of graphene armchair (AC) and zigzag (ZZ) edges were calculated as 3.00 and 1.94 eV, respectively; thus the ZZ edge grows faster than the AC one. Our theory successfully explained why the circumference of a graphene island grown on insulating substrates is generally dominated by AC edges, which is a long-standing puzzle of graphene growth. In addition, the very slow graphene growth rate on an insulating substrate is calculated and agrees well with existing experimental observations. The comprehensive insights on the graphene growth on insulating surfaces at the atomic scale provide guidance on the experimental design for high-quality graphene growth on insulating substrates.