Multilayer Graphene Research Articles

Graphite and multi-layer graphene from a low molecular weight carbon source

While carbonaceous structures formed by pyrolysis of macromolecular carbon sources with silicates are well described in the literature, information on the structure of carbons obtained in the similar way from low molecular weight (LMW) carbon sources is not sufficient. This study is therefore aimed at characterizing the material obtained by pyrolyzing (1300 °C; Ar atmosphere) montmorillonite containing ∼25-50 wt.% LMW cations as a carbon source. Pyrolyzed samples contained ∼5-20 wt.% carbon, and thermogravimetric and elemental analysis showed a higher yield for a higher original amount of the LMW carbon source. In addition to amorphous carbon, graphite was formed during pyrolysis, as confirmed by X-ray diffraction analysis, Raman spectroscopy, and X-ray photoelectron spectroscopy. The presence of graphene-based nanomaterial, specifically multi-layer graphene, was revealed by transmission electron microscopy (TEM). Electrical conductivity of the silicate/carbon material reached ∼35 S·m-1. Raman spectra and TEM images are similar to those from studies describing the use of macromolecular carbon sources. LMW compounds are a sufficient source of carbon for the preparation of electrically conductive materials containing graphite and multi-layer graphene.

Charge-Selective 2D Heterointerface-Driven Multifunctional Floating Gate Memory for In Situ Sensing-Memory-Computing.

Flash memory, dominating data storage due to its substantial storage density and cost efficiency, faces limitations such as slow response, high operating voltages, absence of optoelectronic response, etc., hindering the development of sensing-memory-computing capability. Here, we present an ultrathin platinum disulfide (PtS2)/hexagonal boron nitride (hBN)/multilayer graphene (MLG) van der Waals heterojunction with atomically sharp interfaces, achieving selective charge tunneling behavior and demonstrating ultrafast operations, a high on/off ratio (108), extremely low operating voltage, robust endurance (105 cycles), and retention exceeding 10 years. Additionally, we achieve highly linear synaptic potentiation and depression, and observe the reversibly gate-tunable transitions between positive and negative photoconductivity. Furthermore, we employed the VGG11 neural network for in situ trained in-sensor-memory-computing to classify the CIFAR-10 data set, pushing accuracy levels comparable to pure digital systems. This work could pave the way for seamlessly integrated sensing, memory, and computing capabilities for diverse edge computing.

New Comprehensive Stability and Sensitivity Analysis on Graphene Nanoribbon Interconnects Parameters

Based on the transmission line modeling for multilayer graphene nanoribbon (MGNR) interconnects, system stability was studied on intrinsic parameters. In addition to width,length and height variation, dielectric constant, permeability and Fermi velocity path change in multilayer graphene nanoribbon (MGNR) interconnects are analyzed. In thispaper, the obtained results show with increasing dielectric constant and decreasing permeability, Fermi velocity system becomes more stable. Nyquist diagram and stepresponse method results confirm these and are matched with physical parameter variation like resistance, capacitance and inductance in the following sensitivity analysis results where it shows with increasing width and length, sensitivity will decrease and increase respectively. Impulse response diagram results show with increasing 50% width, sensitivity will be zero but with increasing 50% length, amplitude will decrease and the time of setting will increase. On the other hand, from the step response of the transfer function, both width and length increase cause more stability for a system but the width parameter will be a better choice for manipulating the dimension of MGNR to reach a stable system.

Optical properties of CVD-grown multilayer graphene on nickel using spectroscopic ellipsometry

Incorporating graphene into relevant technologies requires its integration with commercially suitable substrates. Understanding the interactions between graphene and these substrates is crucial, as graphene serves as an ideal model system for investigating electronic phenomena. In this work, we report the optical properties of multilayer graphene on nickel substrates using spectroscopic ellipsometry. We provide information on the spectral dependence of optical properties of multilayer graphene, such as the complex dielectric constant, refractive index, and optical conductivity in the energy range of 1.6–5.0 eV. The optical conductivity profile obtained from SE analysis showed a symmetrical peak at 4.38 eV, suggesting an interband transition from the π to π∗ orbital at the M point. The graphene/Ni interaction generated changes in the number of available states below the Fermi level, leading to significant changes in electron density. Our result provides the information essential for understanding relevant research and developing graphene-based optoelectronic applications.

Vibration analysis of multilayer graphene origami-enabled metamaterial plates

Vibration analysis of multilayer graphene origami-enabled metamaterial plates

One-Selector-One-Resistor Integrated Memory Cells Based on Two-Dimensional Heterojunction Memory Selectors.

Selectors are critical components for reducing the sneak path leakage currents in emerging resistive random-access memory (RRAM) arrays. Two-dimensional (2D) materials provide a rich choice of materials with van der Waals stacking to form the heterostructure selectors with controllable energy barriers. Here, we experimentally demonstrate 2D-material-based heterostructure selectors with exponential current-voltage (I-V) relationships and integrate them with hafnium oxide (HfOx)-based RRAMs, forming one-selector-one-resistor (1S1R) cells. The multilayer graphene (MG)/tungsten disulfide (WS2)/platinum (Pt) selector contains two asymmetric heterojunctions with different Schottky barriers, which lead to highly nonlinear and asymmetric I-V characteristics. The 2D selectors in 1S1R cells can successfully drive RRAMs, reduce sneak path leakage current by more than 100 times, and provide the set compliance current. The 1S1R cells are further modeled and integrated into both planar and 3D memory arrays, with circuit-level simulations demonstrating that the presence of 2D selectors in large memory arrays can reduce the power consumption by up to 86%, improve the read/write margin by up to 31%, and avoid write failure. Such a platform holds high potential for constructing 3D high-density memories and performing in-memory computing.

RF NEMS switches based on graphene for low pull-in voltage and excellent RF performance

This study introduces a novel graphene RF NEMS capacitive switch and conducts an extensive analysis of its RF performance using CST and COMSOL Multiphysics software. The switch’s characteristic impedance matching is accomplished through a coplanar waveguide (CPW) structure, incorporating a dielectric layer topped with conductive graphene beam electrodes. Simulation results reveal that the monolayer graphene RF NEMS switch maintains an insertion loss of 0.003 ~ 0.015 dB and an isolation greater than 40 dB across an ultra-wideband (UWB) frequency range of DC ~ 140 GHz. Moreover, the switch demonstrates a switching time of 4.03 ps at a pull-in voltage of 1 V. The performance of multilayer graphene RF NEMS switches was also evaluated. The study further investigates the operational mechanism of the graphene RF NEMS switch and performs finite element analysis on the proposed design. The graphene RF NEMS switch discussed herein offers significant advantages, including minimal size, lightweight, cost-effectiveness, low pull-in voltage, rapid response time, excellent RF performance, and reduced space consumption in circuitry. Its potential applications span a range from L to F bands, encompassing data storage, communication systems, sensors, remote sensing and military uses.

Investigating the role of graphene in the formation and stability of [formula omitted]-phase antimonene islands

Two-dimensional materials have shown tremendous potential for various technological applications. Particularly, 2D antimony exhibits high applicability in electronics, sensors, and batteries. This 2D material, known as antimonene, presents two stable phases: α (rectangular lattice) and β (honeycomb lattice), whose formation depends on the substrate where antimony is deposited. In this study, we investigated the growth of antimonene islands on graphene, forming an antimonene/graphene heterostructure. To demonstrate the significance of graphene in the synthesis of antimonene, we also studied antimony deposited on a bare copper foil similar to the one used for the graphene substrate. Antimony deposition exhibits the β phase antimonene structure when deposited on top of monolayer graphene, but not when deposited on a bare copper foil, nor on top of multilayer graphene. Additionally, we investigated the stability of the heterostructure after exposure to air. Pure antimony islands are formed when evaporated in high vacuum on top of graphene and copper substrates, and antimony atoms oxidize upon exposure to air. After annealing the sample in ultra-high-vacuum at temperatures lower than 200 °C, more than half of pure antimony is recovered and almost all oxidized antimony is desorbed from the graphene substrate. In contrast, almost none of the oxidized antimony is desorbed from the bare copper substrate, highlighting the key role of the heterostructure on the formation and preservation of the physical and chemical properties of the deposited 2D material.

Enhanced Growth of Homogeneous Multilayer Graphene on Ni(111) via Airflow Microcavity-Assisted PECVD

Enhanced Growth of Homogeneous Multilayer Graphene on Ni(111) via Airflow Microcavity-Assisted PECVD

Influence of dislocations in multilayer graphene stacks: A phase field crystal study

Influence of dislocations in multilayer graphene stacks: A phase field crystal study

A Versatile Metal-Organic-Framework Pillared Interlayer Design for High-Capacity and Long-Life Lithium-Sulfur Batteries.

Developing high-performance lithium-sulfur batteries is a promising way to attain higher energy density at lower cost beyond the state-of-the-art lithium-ion battery technology. However, the major issues blocking their practical application are the sluggish kinetics and parasitic shuttling reactions for sulfur and polysulfides. Here, pillaring multilayer graphene with the metal-organic framework (MOF) demonstrates the substantial impact of a versatile interlayer design in tackling those issues. Unlike regular composite separators reported so far, the participation of tri-metallic Ni-Co-Mn MOF (NCM-MOF) as pillars supports the construction of an ion-channel interconnected interlayer structure, unexpectedly balancing the interfacial concentration polarization, spatially confining the soluble polysulfides and vastly affording lithiophilic sites for highly efficient polysulfide sieving/conversion. As a demonstration, we show that the MOF-pillared interlayer structure enables outstanding capacity (1634 mAh g-1 at 0.1C) and longevity (average capacity decay of 0.034% per cycle in 2000 cycles) of lithium-sulfur batteries. Besides, the multilayer separator can be readily integrated into the high-nickel cathode (LiNi0.91Mn0.03Co0.06O2)-based lithium-ion batteries, which efficiently suppresses the undesired phase evolution upon cycling. These findings suggest the potential of "gap-filling" materials in fabricating multi-functional separators, bring forward the pillared interlayer structure for energy-storage applications.

A Versatile Metal‐Organic‐Framework Pillared Interlayer Design for High‐Capacity and Long‐Life Lithium‐Sulfur Batteries

Developing high‐performance lithium‐sulfur batteries is a promising way to attain higher energy density at lower cost beyond the state‐of‐the‐art lithium‐ion battery technology. However, the major issues blocking their practical application are the sluggish kinetics and parasitic shuttling reactions for sulfur and polysulfides. Here, pillaring multilayer graphene with the metal‐organic framework (MOF) demonstrates the substantial impact of a versatile interlayer design in tackling those issues. Unlike regular composite separators reported so far, the participation of tri‐metallic Ni‐Co‐Mn MOF (NCM‐MOF) as pillars supports the construction of an ion‐channel interconnected interlayer structure, unexpectedly balancing the interfacial concentration polarization, spatially confining the soluble polysulfides and vastly affording lithiophilic sites for highly efficient polysulfide sieving/conversion. As a demonstration, we show that the MOF‐pillared interlayer structure enables outstanding capacity (1634 mAh g‐1 at 0.1C) and longevity (average capacity decay of 0.034% per cycle in 2000 cycles) of lithium‐sulfur batteries. Besides, the multilayer separator can be readily integrated into the high‐nickel cathode (LiNi0.91Mn0.03Co0.06O2)‐based lithium‐ion batteries, which efficiently suppresses the undesired phase evolution upon cycling. These findings suggest the potential of “gap‐filling” materials in fabricating multi‐functional separators, bring forward the pillared interlayer structure for energy‐storage applications.

Mechanical and tribological properties of high entropy carbide-based micro-nano ceramic composites

(NbTaTiWZr)C-based micro-nano composites were fabricated by spark plasma sintering employing multi-layer graphene (MLG), Ni, and Al2O3 as reinforcements. It is demonstrated that excellent mechanical properties were achieved for MLG, Ni, and Al2O3 hybrid addition with a hardness of 21.73 GPa, a flexural strength of 572.4 MPa, and a fracture toughness of 7.65 MPa m1/2. Enhanced densification together with inhibited grain growth contributed to the simultaneously improved hardness and flexural strength. The major toughening mechanisms were determined as microcracks, crack deflection, crack bridging, crack stopping, MLG wall, MLG pull-out, MLG bending, and MLG wrapping grains. Furthermore, outstanding tribological performance occurred to the (High entropy ceramic) HEC-Ni-Al2O3-MLG with a friction coefficient of 0.23 and wear rate of 4.32 × 10−7mm3N−1m−1, as a function of graphene acting as a lubricating friction layer and the enhanced mechanical responses.

Preparation and growth mechanism of high-quality multilayer graphene from simulated coal pyrolysis gas via chemical vapor deposition

Chemical vapor deposition (CVD) of graphene from coal pyrolysis gas provides new ways for both large-scale graphene preparation and high value-added utilization of coal. However, green, efficient and continuous preparation of high-quality multilayer graphene with both good uniformity and ideal structure characteristic remains a great challenge. Herein, we first investigated the influence of main carbonaceous species (CH4, C2H6, C3H8, CO2, and CO) in coal pyrolysis gas on the quality of CVD graphene products. The experimental results indicated that CO2 and CO have little effect on the growth of graphene, while methane as carbon source is conducive to obtain ideal graphene materials, propane and ethane could also influence structural defects and layer number of graphene products remarkably. On this basis, we designed a mixed gas of methane, ethane, and propane with optimized ratio as simulated coal pyrolysis gas, and successfully prepared high-quality multilayer graphene products on nickel foam from the as-designed simulated coal pyrolysis gas by CVD method. Notably, with a CH4:C2H6:C3H8 ratio of 2:1:1, the graphene products prepared from simulated coal pyrolysis gas outperformed that of raw coal pyrolysis gas in terms of physical structure, layer number, and quality uniformity. The corresponding I2D/IG value reached 0.97. The graphene growth process and mechanism were investigated and discussed macroscopically and microscopically. This work is of great significance for the intrinsic understanding of CVD growth of graphene from coal pyrolysis gas, and also inspires an efficient and environmentally friendly avenue for high-throughput, uniform production of high-quality graphene materials.

Atomic scale analysis of sub-10 nm implantation of size-selected gold clusters into multilayer graphene

Atomic scale analysis of sub-10 nm implantation of size-selected gold clusters into multilayer graphene

High-value multilayer graphene oxide prepared by catalytic pyrolysis of petroleum tar and applications: Trash to treasure

Petroleum tar (PT), a by-product of heavy oil refining, poses significant environmental challenges due to its high production volume and associated pollution risks. This study presents an innovative approach for the catalytic conversion of PT into multilayer graphene oxide using nickel foam (NiF) as a catalyst at reaction temperatures of 500 °C and 700 °C (GT/Ni500 and GT/Ni700). The process effectively decomposes PT and facilitates the structured rearrangement of carbon atoms into graphene layers. Comprehensive characterization techniques, including SEM-EDS, HRTEM, BET, XRD, XPS, and Raman spectroscopy, confirm the formation of high-quality graphene oxide. The synthesized GT/Ni700 material exhibits remarkable electrochemical performance with a specific capacitance of 3.34F/g. GT/Ni500 shows adsorption capacities of 59.86 mg/g for Pb2+ and 56.84 mg/g for Cu2+. Life Cycle Assessment reveals a substantial reduction in the carbon footprint, with CO2 equivalents for GT/Ni500 and GT/Ni700significantly lower than traditional methods, at 17.64 kg/CO2eq and 14.03 kg/CO2eq, respectively, representing a reduction of over 50 %. This study not only offers a sustainable pathway for PT utilization but also provides advanced materials with dual utility in electrochemical applications and heavy metal adsorption, contributing to environmental remediation and reducing reliance on non-renewable resources.

Antiscreening and Nonequilibrium Layer Electric Phases in Graphene Multilayers.

Screening is a ubiquitous phenomenon through which the polarization of bound or mobile charges tends to reduce the strengths of electric fields inside materials. Here, we show how photoexcitation can be used as a knob to transform conventional out-of-plane screening into antiscreening-the amplification of electric fields-in multilayer graphene. We find that, by varying the photoexcitation intensity, multiple nonequilibrium screening regimes can be accessed, including near-zero screening, antiscreening, and overscreening (reversing electric fields). Strikingly, at modest continuous wave photoexcitation intensities, the nonequilibrium polarization states become multistable, hosting light-induced ferroelectriclike steady states with nonvanishing out-of-plane polarization (and band gaps) even in the absence of an externally applied displacement field in nominally inversion symmetric stacks. This rich phenomenology reveals a novel paradigm of dynamical quantum matter that we expect will enable a variety of nonequilibrium broken symmetry phases.

Utilizing synergy of MLG and MWCNT with optimized mixing protocol to improve the high temperature stability of SBS modified bitumen

High temperature instability is the biggest problem which limits the application of Styrene-Butadiene-Styrene (SBS) modified bitumen in flexible pavements. Addition of multi-layer graphene (MLG) nanomaterial improves the performance of SBS modified bitumen, but deteriorates its thermal stability. The binary additive comprising of MLG and multi-walled carbon nanotubes (MWCNT) can be a way to improve the thermal stability through their synergistic effects, however, mixing protocol needs to be optimized simultaneously. In this present study, MLG, MWCNT and their combination have been dispersed by two different organic solvent dissolution protocols, i.e., wet and dry to prepare the SBS-nano modified binders. Thermal stability analysis and rheological characterization (small & large amplitude oscillatory shear) have been used to optimize the method and to compare the effect of sole and binary additive. Advanced tools such as Raman spectroscopy and Field emission scanning electron microscopy have been used to understand the underlying science at micro-molecular level. The synergistic effects of combined additives are prominently visible only in dry organic dissolution method and with this method, the combination of MLG-MWCNT (0.1phr-1phr) significantly eliminates the thermal instability of SBS modified binder by upto 96 %. This SBS-nano modified bitumen may serve as futuristic binder for the black top pavements.

Microstructural design of crown nanopores in graphene membrane for efficient desalination process

Designing a membrane with simultaneous high water permeability and desalination rate to overcome the trade-off presents a persistent and substantial challenge. In this paper, we employed molecular dynamics simulations to design the structure of the graphene crown ether reverse osmosis membrane and elucidate the relationship between the membrane's microscopic separation mechanism and its structure-activity.The results show that the water permeability through crown graphene nanopores exceeded that of the original graphene nanopores by an order of magnitude, and hundreds of times greater than that of the traditional reverse osmosis membrane. Additionally, the water permeation in multilayer crown graphene nanopores also surpassed that in monolayer original graphene nanopores. The water permeability exceeds 46.73 L/cm2/day/Mpa with 100 % salt rejection. Furthermore, the various sizes and shapes of graphene nanopores significantly influence water permeation. Within crown graphene nanopores, a narrow pore enables superior water permeation and salt rejection compared to a circular shape, unlike original graphene nanopores. Observed from MD simulation trajectories,this highly water permeation is caused by the hydrogen bonding between crown ether graphene and water molecules. First-principle calculations further confirm that water transport in graphene crown ether is energetically more favorable than in original graphene nanopores. Our findings support crown graphene membranes as promising candidates for seawater desalination.

Correlation effect between the capillary flow and evaporation rate of water in a 2-D photothermal membrane

To shed light on the correlation effect between the capillary flow and phase transition of water in photothermal evaporation, the non-equilibrium molecular dynamics (NEMD) simulations were employed to investigate the evaporation of water in Multilayered graphene oxide membranes. It was initially found that water molecules need to overcome strong energy barriers to migrate upward by layers before evaporation, with the energy barrier increasing with the reduction in nanogap, hydroxyl content, or increase in layer spacing of graphene sheets. The strong energy barrier accordingly results in dramatic sensible heat conversion and high evaporation temperature. It was shown that the enhanced temperature and hydrophilicity both weaken the hydrogen bond strength of water molecules confined in 2-dimensional channels, contributing to the reduced evaporation enthalpy. The preferential pathways in graphene channels or the weakened hydrogen bonds in hydroxyl-functionalized graphene of water molecules were found to be important influences on capillary flow energy consumption, leading to differences in evaporation energy supply. In combination with these effects, the evaporation rate could be increased by up to 2 folds and an interfacial enthalpy of evaporation below 1500 kJ kg−1 could be achieved by properly tuning the configuration and chemical properties of the graphene membrane. Our findings lay a theoretical foundation for providing a strategy to improve the interfacial evaporation performance in desalination.