Flexible Graphene Research Articles

Conformational interlocking induced construction of hierarchically porous graphene membrane for ultrahigh-pressure sensing

Based on microstructure engineering, graphene oxide (GO)-based piezoresistive pressure sensors have attracted increasing attention due to its amazing sensitivities, but the point-to-point contact mechanism among nanosheets compromises their high-pressure monitoring capabilities. Inspired by the multiple conformations of GO nanosheets, we utilize π-π conjugated interlayer interactions to lock the 3D crumpled conformation of nanosheets, resulting in controllable assembly into a flexible graphene membrane with hierarchically porous structures (PGM). These designed structures include microscale pores formed by the loose stacking of 3D crumpled nanosheets and nanoscale pores supported by densely packed crumples, reaching up to 100 nm in height. The PGM flexible sensor exhibits an unprecedented ultrahigh-pressure response of up to 2000 kPa, with high sensitivities of 1.1 and 0.7 kPa−1 in the pressure ranges of 1–600 kPa and 600–2000 kPa, respectively, and demonstrates over 10,000 cycles of high-pressure stability. Moreover, the PGM flexible sensors enable real-time monitoring of pressure vessel inflation/deflation processes and human activities such as finger, elbow, and knee bending, as well as walking, running, and jumping. This hierarchically porous structure provides a promising avenue for ultra-wide-range and ultra-high-pressure sensing devices, with potential applications in structural health monitoring, personal healthcare, and medical diagnostics.

Properties of Multistranded Twisted Graphene Fibers and Their Application in Flexible Light-Emitting Devices.

As a typical carbon-based material electrode, graphene fiber exhibits many advantages, such as good electrical conductivity, lightweight, and strong structural designability. Its demand is increasing in the wearable display field. With the help of fine denier fiber spinning combined with multistranded graphene fibers prepared via twisting and drafting, their petal-like twisted structure endows the fibers with a high specific surface area, enabling them to complete dye adsorption within 30 min. Simultaneously, compared with that of a single fiber with the same thickness, the volume specific resistance of a multistranded twisted graphene fiber is reduced by 2.4 times. During force sensing, the twisted structure of multistranded fibers exhibits varying simultaneity of fiber fracture with excellent resistance sensitivity reaching up to 55%. The multistranded twisted flexible graphene fibers demonstrate excellent robustness. Electroluminescent flexible devices prepared with graphene fibers and fiber braided fabrics with different organizational structures as electrodes emit highly saturated short-wave blue light during long-term multiple use. Therefore, multistranded twisted graphene fibers exhibit considerable potential for future applications in wearable multicolor smart displays and flexible optical signal electronics.

Free-standing graphene oxide/carboxymethyl cellulose paper-based triboelectric nanogenerator for self-powered motion sensor

Triboelectric nanogenerators (TENG) are innovative energy-harnessing devices that serve as potential power sources for small portable electronics, operating on the principle of electrostatic induction. In this study, we demonstrate the fabrication of paper-like flexible graphene oxide/carboxymethyl cellulose (GO/CMC) composite film and their use as a tribo-positive layer in the TENG with fluorinated ethylene propylene (FEP) film as the tribo-negative layer. The GO/CMC TENG possesses high-energy harvesting performance compared to the bare CMC-based TENG that is due to the increase in surface charge of CMC due to the inclusion of GO sheets, as analyzed using Kelvin probe force microscopy (KPFM). The GO/CMC TENG device demonstrates an output voltage of 97 V and a short-circuit current of 1.2 µA, achieving a peak power of 41.4 µW, notably higher compared to state-of-the-art TENG devices. As a proof-of-concept, we also demonstrated the practical applicability of the GO/CMC TENG in day-to-day life for monitoring the human body motions and to drive portable electric devices, which ensures their candidature towards next-generation self-powered systems.

Study on Confined Water in Flexible Graphene/GO Nanochannels.

The structural evolution of flexible nanochannels within a 2D material membrane, influenced by the ingress of water molecules, plays a crucial role in the membrane's filtration and structural stability. However, the experimental observation of nanoscale water is challenging, and current studies mostly focus on rigid nanochannels. Further investigation on the nanoconfined water is urgently needed, considering the flexibility and deformation of the channel. In this work, MD simulations and theoretical analyses are conducted to investigate the water structure and thermodynamic properties when confined within both rigid and flexible graphene/graphene oxide (GO) nanochannels. In free rigid graphene nanochannels, the interlayer distance exhibits a quantized increase with the number of water molecules, along with sudden changes in entropy, potential energy, and free energy of the water molecules. Meanwhile, in flexible graphene nanochannels, the average interlayer space increases linearly with the number of water molecules. In free rigid GO nanochannels, with the increase of oxidation concentration, the quantized increase in the interlayer space gradually diminishes, accompanied by a decrease in both potential energy and free energy. This work provides insights into the configurational evolution of flexible nanochannels within water, offering guidance in fields such as desalination and mass transport of 2D material membranes.

Multifunctional and high‐stability RGO/PANI wrapped polyurethane foam for flexible piezoresistive sensor applications

AbstractDue to its excellent durability and steady mechanical qualities, three‐dimensional porous polyurethane foam (PUF) presents a wide range of possibilities for flexible piezoresistive sensors. Its extreme flammability, poor electrical conductivity, and susceptibility to outside factors present serious difficulties, though. In this study, a waterborne polyurethane‐coated flexible PUF sensor that incorporates reduced graphene oxide (RGO) and polyaniline (PANI) through a methodical, step‐by‐step dip‐coating methodology is successfully developed. The final product has a water contact angle of 133°, which improves its ability to adapt to a variety of environmental circumstances. Flexible graphene sheets are incorporated to improve heat resistance and flame retardancy, and PANI and RGO provide strong bonding to the PUF framework, ensuring outstanding structural stability even after 1500 cycles. The flexible foam sensor shows promise for use in flexible piezoresistive sensors and electronic skin due to its remarkable strain monitoring range of up to 70%, quick response time of 0.39 s in sensitivity experiments, and adaptability to different physical activities like walking and gesturing.

Wet-Spinning Assembly of Flexible, Ultratough, and Conductive Alkali Lignin Functionalized Graphene Oxide Composite Fibers for Fiber-Shaped Supercapacitor

Wet-Spinning Assembly of Flexible, Ultratough, and Conductive Alkali Lignin Functionalized Graphene Oxide Composite Fibers for Fiber-Shaped Supercapacitor

High mobility graphene field effect transistors on flexible EVA/PET foils

Monolayer graphene is a promising material for a wide range of applications, including sensors, optoelectronics, antennas, EMR shielding, flexible electronics, and conducting electrodes. Chemical vapor deposition (CVD) of carbon atoms on a metal catalyst is the most scalable and cost-efficient method for synthesizing high-quality, large-area monolayer graphene. The usual method of transferring the CVD graphene from the catalyst to a target substrate involves a polymer carrier which is dissolved after the transfer process is completed. Due to often unavoidable damage to graphene, as well as contamination and residues, carrier mobilities are typically 1000–3000 cm2(Vs)−1 , unless complex and elaborate measures are taken. Here, we report on a simple scalable fabrication method for flexible graphene field-effect transistors that eliminates the polymer interim carrier, by laminating the graphene directly onto office lamination foils, removing the catalyst, and depositing Parylene N as a gate dielectric and encapsulation layer. The fabricated transistors show field- and Hall-effect mobilities of 7000–10 000 cm2(Vs)−1 with a residual charge-carrier density of 2×1011 1 cm−2 at room temperature. We further validate the material quality by terahertz time-domain spectroscopy and observation of the quantum Hall effect at low temperatures in a moderate magnetic field of ∼5 T. The Parylene encapsulation provides long-term stability and protection against additional lithography steps, enabling vertical device integration in multilayer electronics on a flexible platform.

Self-Powered cobalt nanocluster decorated flexible graphene based Tribo-Sensors for respiratory diagnosis of critical asthma patient

Self-powered ultrafast sensors have received much attention for sustainable operation without any external power source in the Internet of Things (IoT) platform. This paper proposes faster responsive, highly sensitive triboelectric nanogenerator (TENG) sensors based on few layered nitrogen-doped graphene anchored with cobalt nanocluster (Co-N-Gr) to detect the relative concentration of target species, their proximity analysis, and monitor malfunction of human respiration in real-time. Herein, to understand the sensing mechanism, P-type behaviour of this active material is verified under the FET platform by reducing the leakage current density via the implementation of dual dielectric gate (NiO (200 nm)-SiO2 (10 nm)) oxides leading to better control over channel mobility. The device exhibits maximum sensitivity of around 4722 % at zero bias conditions with excellent response and recovery time of 1.16 s and 1.39 s, respectively which falls within the range of standard human breathing frequency. The triboelectric nature of the sensor device at 1 V bias under natural breathing exhibits a high sensitivity (39.56 %) towards relative humidity of 10–90 % with excellent stability over 13 h. In addition, our TENG sensor is highly sensitive towards NOx content upto ppb levelwhich can improve reliability towards asthma detection as NOx content is relatively higher in asthma patients. This approach provides an integrated platform not only towards selective detection of NOx content as well as to identify the individual breathing strength. Furthermore, as-fabricated self-powered device demonstrates its potential in differentiating various respiratory status and has the capability to detect acute exacerbation of chronic obstructive pulmonary disease (AECOPD) via a distinct pattern recognition. Therefore, the work paves the way to design a low-cost flexible device fabrication on Kapton substrate integrable with wearable appliances for commercialization.

Synergy of modulating in-plane pores and zincophilic sites on the flexible graphene paper for efficient and dendrite-free hosted Zn anode

The practical advancement of Zn-ion batteries (ZIBs) in the portable/wearable electronics field is still hindered by the notorious Zn dendrites formation and the lack of an appropriate host to construct a highly effective flexible Zn anode. Herein, we present a three-dimensional (3D) N-doped graphene paper framework with abundant in-plane pores (rHGP-N) as an efficient Zn plating/stripping scaffold. Remarkably, the rHGP-N paper electrode exhibits an unprecedentedly low Zn nucleation overpotential of 5.2 mV and maintains a high average Coulombic efficiency (∼99.3%) over a superior long Zn plating/stripping cycling of 1400 h. DFT calculation results demonstrate that pyrrolic-nitrogen on graphene possesses the strongest adsorption energy for Zn2+, serving as zincophilic sites to guide Zn uniform nucleation. Moreover, the finite elements simulation results illustrate that flexible graphene paper with abundant in-plane pores can mitigate structural stress and inhibit the formation of Zn dendrites by spatially homogenizing Zn2+ ions flux throughout the entire electrode. The assembled ZIBs full cell (rHGP-N@Zn//rHGP-N@Mn3(PO4)2) demonstrates an impressive volumetric energy density of 77 mWh/cm3, as well as excellent flexibility and mechanical stability with negligible capacity decay under harsh deformation conditions. Our approach can be potentially utilized in designing dendrite-free metal-based flexible anodes for Mg, Ca, or Al-ion batteries.

Highly Flexible and Superelastic Graphene Nanofibrous Aerogels for Intelligent Sign Language.

Highly flexible and superelastic aerogels at large deformation have become urgent mechanical demands in practical uses, but both properties are usually exclusive. Here a trans-scale porosity design is proposed in graphene nanofibrous aerogels (GNFAs) to break the trade-off between high flexibility and superelasticity. The resulting GNFAs can completely recover after 1000 fatigue cycles at 60% folding strain, and notably maintain excellent structural integrity after 10000 cycles at 90% compressive strain, outperforming most of the reported aerogels. The mechanical robustness is demonstrated to be derived from the trans-scale porous structure, which is composed of hyperbolic micropores and porous nanofibers to enable the large elastic deformation capability. It is further revealed that flexible and superelastic GNFAs exhibit high sensitivity and ultrastability as an electrical sensors to detect tension and flexion deformation. As proof, The GNFA sensor is implemented onto a human finger and achieves the intelligent recognition of sign language with high accuracy by multi-layer artificial neural network. This study proposes a highly flexible and elastic graphene aerogel for wearable human-machine interfaces in sensor technology.

Flexible laser-induced graphene electrodes on polyimide film: Hybrid nanoflower-modified dielectric microjunctions for non-faradaic analysis

Laser-induced Graphene (LIG) electrodes on flexible substrates have attracted significant research interest, making them an excellent alternative to conventional fabrication of transducers on rigid planar substrates. In this study, four individual capacitor-like triangular LIG electrodes were fabricated on polyimide (PI) film with micron gap (MG) spacing of 30, 66, 125 and 180 µm, to study the relationship between gap spacing and capacitance. A novel N, N-carbonyldiimidazole-copper (CDI-Cu) hybrid nanoflower (NF) was synthesised via one-pot biomineralization and deposited at the triangular junction of acid-base treated LIG-MG for the immobilization of neutravidin. The gap spacing and structure of the LIG-MG were analysed using high-resolution microscopes, revealing a porous nanofiber-like graphene structure. X-ray Photoelectron Spectroscopy (XPS) of acid-base treated PI film proved carboxyl group formation. A decrease in capacitance was observed with an increasing gap spacing in a non-faradaic environment. The capacitance of CDI-Cu NF following neutravidin modification for 30, 66, 125 and 180 µm spacings were 1.77E-07, 1.36E-07, 4.73E-08, 4.84E-08 F, respectively, suggesting excellent biomolecular modification sensitivity of the LIG-MG with 30 µm spacing. A comparative analysis of dielectric performance for different gap-spaced devices revealed that a 30 µm spacing would be optimal for bio-capturing because of the close confinement of biomolecules for smaller gapped areas.

A Large-Scale and Low-Cost Thermoacoustic Loudspeaker Based on Three-Dimensional Graphene Foam.

Graphene is a promising material for thermoacoustic sources due to its extremely low heat capacity per unit area and high thermal conductivity. However, current graphene thermoacoustic devices have limited device area and relatively high cost, which limit their applications of daily use. Here, we adopt a dip-coating method to fabricate a large-scale and cost-effective graphene sound source. This sound source has the three-dimensional (3D) porous structure that can increase the contact area between graphene and air, thus assisting heat to release into the air. In this method, polyurethane (PU) is used as a support, and graphene nanoplates are attached onto the PU skeleton so that a highly flexible graphene foam (GrF) device is obtained. At a measuring distance of 1 mm, it can emit sound at up to 70 dB under the normalized input power of 1 W. Considering its unique porous structure, we establish a thermoacoustic analysis model to simulate the acoustic performance of GrF. Furthermore, the obtained GrF can be made up to 44 in. (100 cm × 50 cm) in size, and it has good flexibility and processability, which broadens the application fields of GrF loudspeakers. It can be attached to the surfaces of objects with different shapes, making it suitable to be used as a large-area speaker in automobiles, houses, and other application scenarios, such as neck mounted speaker. In addition, it can also be widely used as a fully flexible in-ear earphone.

Engineering lightweight Poly(lactic acid) graphene nanoribbon nanocomposites for sustainable and stretchable electronics: Achieving exceptional electrical conductivity and electromagnetic interference shielding with enhanced thermal conductivity

The challenge of creating flexible and sustainable electronics with properties such as lightweight, electrical and thermal conductivity, and electromagnetic interference (EMI) shielding is addressed in this study. Carbon nanotubes and graphene are commonly used in flexible electronic devices, but gaps exist in their conductivity and flexibility. A novel and scalable fabrication method is introduced, involving the creation of bio-based nanocomposites by integrating flexible and high aspect-ratio graphene nanoribbons (GNRs) into a poly (lactic acid) (PLA) matrix. The nanocomposites were drawn above the glass transition temperature (Tg) of PLA, resulting in the formation of extended shish structures, as observed in scanning electron microscope (SEM) images. These structures significantly enhanced thermal and electrical conductivities, as well as EMI shielding features. The combination of flexible GNR nanofillers with uniaxial stretching led to a substantial increase in Young's modulus, tensile strength, and toughness by approximately 550 %, 440 %, and 600 %, respectively, most likely due to the increased network connection despite the higher flexibility of GNRs. Moreover, in-plane thermal conductivity registered a notable enhancement of approximately 110 %. The EMI shielding reached 26 dB, with an absorption contribution to EMI shielding of around 45 %. Additional improvement was achieved through foaming of the stretched samples, resulting in multilayer structures with alternative extended shish and foam structures. Furthermore, a significant augmentation of approximately 33 dB in total EMI shielding of the foamed samples, accompanied by an 85 % increase in SEA was documented. These promising findings underscore potential applications across diverse domains, including thermal interface materials, electronic packaging, capacitors, and energy storage devices, with a specific emphasis on the realm of sustainable and stretchable electronics.

Staggered structural dynamic-mediated selective adsorption of H2O/D2O on flexible graphene oxide nanosheets

Graphene oxide (GO) is the one of the most promising family of materials as atomically thin membranes for water-related molecular separation technologies due to its amphipathic nature and layered structure. Here, we show important aspects of GO on water adsorption from molecular dynamics (MD) simulations, in-situ X-ray diffraction (XRD) measurements, and ex-situ nuclear magnetic resonance (NMR) measurements. Although the MD simulations for GO and the reduced GO models revealed that the flexibility of the interlayer spacing could be attributed to the oxygen-functional groups of GO, the ultra-large GO model cannot well explain the observed swelling of GO from XRD experiments. Our MD simulations propose a realistic GO interlayer structure constructed by staggered stacking of flexible GO sheets, which can explain very well the swelling nature upon water adsorption. The transmission electron microscopic (TEM) observation also supports the non-regular staggered stacking structure of GO. Furthermore, we demonstrate the existence of the two distinct types of adsorbed water molecules in the staggered stacking: water bonded with hydrophilic functional groups and “free” mobile water. Finally, we show that the staggered stacking of GO plays a crucial role in H/D isotopic recognition in water adsorption, as well as the high mobility of water molecules.

Graphene Nanocomposite Ink Coated Laser Transformed Flexible Electrodes for Selective Dopamine Detection and Immunosensing.

Novel and flexible disposable laser-induced graphene (LIG) sensors modified with graphene conductive inks have been developed for dopamine and interleukin-6 (IL-6) detection. The LIG sensors exhibit high reproducibility (relative standard deviation, RSD = 0.76%, N = 5) and stability (RSD = 4.39%, N = 15) after multiple bendings, making the sensors ideal for wearable and stretchable bioelectronics applications. We have developed electrode coatings based on graphene conductive inks, poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (G-PEDOT:PSS) and polyaniline (G-PANI), for working electrode modification to improve the sensitivity and limit of detection (LOD). The selectivity of LIG sensors modified with the G-PANI ink is 41.47 times higher than that of the screen-printed electrode with the G-PANI ink modification. We have compared our fabricated bare laser-engraved Kapton sensor (LIG) with the LIG sensors modified with G-PEDOT (LIG/G-PEDOT) and G-PANI (LIG/G-PANI) conductive inks. We have further compared the performance of the fabricated electrodes with commercially available screen-printed electrodes (SPEs) and screen-printed electrodes modified with G-PEDOT:PSS (SPE/G-PEDOT:PSS) and G-PANI (SPE/G-PANI). SPE/G-PANI has a lower LOD of 0.632 μM compared to SPE/G-PEDOT:PSS (0.867 μM) and SPE/G-PANI (1.974 μM). The lowest LOD of the LIG/G-PANI sensor (0.4084 μM, S/N = 3) suggests that it can be a great alternative to measure dopamine levels in a physiological medium. Additionally, the LIG/G-PANI electrode has excellent LOD (2.6234 pg/mL) to detect IL-6. Also, the sensor is successfully able to detect ascorbic acid (AA), dopamine (DA), and uric acid (UA) in their ternary mixture. The differential pulse voltammetry (DPV) result shows peak potential separation of 229, 294, and 523 mV for AA-DA, DA-UA, and UA-AA, respectively.

Fabrication of flexible nitrogen-doped graphene micro-supercapacitors by laser-induced self-made precursors

Fabrication of flexible nitrogen-doped graphene micro-supercapacitors by laser-induced self-made precursors

Highly sensitive flexible graphene pressure sensor based on indocalamus leaves’ microstructure

In recent years, high-performance flexible pressure sensors have attracted much attention due to their important application potential in intelligent robotics, wearable electronics, and electronic skin. Here, a wearable pressure sensor with high sensitivity in a large useable range is demonstrated. By utilizing indocalamus leaf as a template, the sensing layer of the sensor was prepared in the form of Graphene films with a bionic composite microstructure. Due to the hierarchical deformation of bionic composite microstructure, the sensor demonstrates high sensitivity and wide detection range at the same time. The sensitivity of sensor is 4.56 kPa−1 (5 Pa-20 kPa), 1.87 kPa−1 (20 Pa-100 kPa) and 0.70 kPa−1 (100 kPa-250 kPa). Therefore, it is not only sensitive to slight pressure as low as 5 Pa but also has a detection limit up to 250 kPa. At the same time, sensor has a short response time of 130 ms. After 1000 pressure cycles, the current change rate of the sensor can still reach 90% of the original. Meanwhile, the flexible pressure sensor could be used for monitoring human physiological signals, such as wrist pulse, voice recognition, and human activities, which shows a broad application prospect.

Flash healing of laser-induced graphene

The advancement of laser-induced graphene (LIG) technology has streamlined the fabrications of flexible graphene devices. However, the ultrafast kinetics triggered by laser irradiation generates intrinsic amorphous characteristics, leading to high resistivity and compromised performance in electronic devices. Healing graphene defects in specific patterns is technologically challenging by conventional methods. Herein, we report the rapid rectification of LIG’s topological defects by flash Joule heating in milliseconds (referred to as F-LIG), whilst preserving its overall structure and porosity. The F-LIG exhibits a decreased ID/IG ratio from 0.84 – 0.33 and increased crystalline domain from Raman analysis, coupled with a 5-fold surge in conductivity. Pair distribution function and atomic-resolution imaging delineate a broader-range order of F-LIG with a shorter C-C bond of 1.425 Å. The improved crystallinity and conductivity of F-LIG with excellent flexibility enables its utilization in high-performance soft electronics and low-voltage disinfections. Notably, our F-LIG/polydimethylsiloxane strain sensor exhibits a gauge factor of 129.3 within 10% strain, which outperforms pristine LIG by 800%, showcasing significant potential for human-machine interfaces.

Flexible Graphene Paper Modified Using Pt&Pd Alloy Nanoparticles Decorated Nanoporous Gold Support for the Electrochemical Sensing of Small Molecular Biomarkers.

The exploration into nanomaterial-based nonenzymatic biosensors with superb performance in terms of good sensitivity and anti-interference ability in disease marker monitoring has always attained undoubted priority in sensing systems. In this work, we report the design and synthesis of a highly active nanocatalyst, i.e., palladium and platinum nanoparticles (Pt&Pd-NPs) decorated ultrathin nanoporous gold (NPG) film, which is modified on a homemade graphene paper (GP) to develop a high-performance freestanding and flexible nanohybrid electrode. Owing to the structural characteristics the robust GP electrode substrate, and high electrochemically catalytic activities and durability of the permeable NPG support and ultrafine and high-density Pt&Pd-NPs on it, the resultant Pt&Pd-NPs-NPG/GP electrode exhibits excellent sensing performance of low detection limitation, high sensitivity and anti-interference capability, good reproducibility and long-term stability for the detection of small molecular biomarkers hydrogen peroxide (H2O2) and glucose (Glu), and has been applied to the monitoring of H2O2 in different types of live cells and Glu in body fluids such as urine and fingertip blood, which is of great significance for the clinical diagnosis and prognosis in point-of-care testing.

Ti3C2Tx/laser-induced graphene-based micro-droplet electrochemical sensing platform for rapid and sensitive detection of benomyl

The design and fabrication of high-performance electrode devices are highly important for the practical application of electrochemical sensors. In this study, flexible three-dimensional porous graphene electrode devices were first facilely fabricated using common laser ablation technique at room temperature. After then, hydrophilic two-dimensional MXene (Ti3C2Tx) nanosheet was decorated on the surface of the laser-induced graphene (LIG), resulting in disposable Ti3C2Tx/LIG electrode devices. After introducing Ti3C2Tx nanosheet, the electrochemical active area, electron transfer ability of LIG electrode device and its adsorption efficiency toward organic pesticide benomyl was significantly boosted. As a result, the fabricated Ti3C2Tx/LIG electrode device exhibited significantly enhanced electrocatalytic activity toward benomyl oxidation. Based on this, a novel and ultra-sensitive electrochemical platform for micro-droplet detection of benomyl was achieved in the range of 10 nM–6000 nM with detection sensitivity of 169.9 μA μM−1 cm−2 and detection limit of 5.8 nM. Considering the low-cost Ti3C2Tx/LIG electrode devices are rarely used for electrochemical analysis, we believed this research work will contribute to exploring the broader application of MXene/LIG electrode devices in the field of electrochemical sensing.