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Flexible electrodes based on conversion-type materials have potential applications in low-cost and high-performance flexible sodium-ion batteries (FSIBs), owing to their high theoretical capacity and appropriate sodiation potential. However, they suffer from flexible electrodes with poor mechanical properties and sluggish reaction kinetics. In this study, freestanding CoS2 nanoparticles coupled with graphene oxides and carbon nanotubes (CoS2/GO/CNTs) flexible films with robust and interconnected architectures were successfully synthesized. CoS2/GO/CNTs flexible film displays high electronic conductivity and superior mechanical properties (average tensile strength of 21.27 MPa and average toughness of 393.18 KJ m-3) owing to the defect bridge for electron transfer and the formation of the π-π interactions between CNTs and GO. In addition, the close contact between the CoS2 nanoparticles and carbon networks enabled by the Co-N chemical bond prevents the self-aggregation of the CoS2 nanoparticles. As a result, the CoS2/GO/CNTs flexible film delivered superior rate capability (213.5 mAh g-1 at 6 A g-1, better than most reported flexible anode) and long-term cycling stability. Moreover, the conversion reaction that occurred in the CoS2/GO/CNTs flexible film exhibited pseudocapacitive behavior. This study provides meaningful insights into the development of flexible electrodes with superior mechanical properties and electrochemical performance for energy storage.
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For Fe-NC systems, high-density Fe-N sites are the basis for high-efficiency oxygen reduction reaction (ORR), and P doping can further lower the reaction energy barrier, especially in the form of metal-P bonding. However, limited to the irregular agglomeration of metal atoms at high temperatures, Fe-P bonds and high-density Fe-N cannot be guaranteed simultaneously. Here, to escape the random and violent agglomeration of Fe species during high-temperature carbonization, triphenylphosphine and 2-methylimidazole with a strong metal coordination capability are introduced together to confine Fe growth. With the aid of such bidirectional coordination, the high-density Fe-N site with Fe-P bonds is realized by in situ phosphorylation of Fe in an Fe-NC system (Fe-P-NC) at high temperatures. Impressively, the content of single-atomically dispersed Fe sites for Fe-P-NC dramatically increases from 2.8% to 65.3% compared with that of pure Fe-NC, greatly improving the ORR activity in acidic and alkaline electrolytes. The theoretical calculation results show that the generated Fe2P can simultaneously facilitate the adsorption of intermediates to Fe-N4 sites and the electron transfer, thereby reducing the reaction energy barrier and obtaining superior ORR activity.
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Traditional metal materials used in electronic devices are often problematic due to issues like bending resistance, oxidation leading to failure, and environmental pollution. To address these challenges, microwave electronic devices are constantly casting around for metal substitute materials with additional characteristics such as flexibility, anticorrosive, and eco-friendly. However, finding suitable materials that are accessible for radiofrequency (RF) applications is a difficult yet promising task. Consequently, a high-performance metasurface antenna based on highly conductive graphene films for satellite communications is developed in this paper. The proposed graphene assembled films (GAFs) have a conductivity of up to 1.13 × 106 S/m. Simulation and measurement results confirm the excellent performance of the designed antenna. Comparative experiments are also conducted on salt spray and mechanical bending between GAF antenna patterns and copper foil counterparts, further demonstrating the outstanding flexible property and corrosion resistance performance of prepared GAFs.
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Currently, metal-organic frameworks (MOFs) have emerged as viable candidates for enduring electrode materials in nonenzyme glucose sensing. However, given the inherent water susceptibility of MOFs and their complete self-reconstruction during the process of electrochemical oxygen evolution in alkaline conditions, we are motivated to explore the truth of MOFs catalyzing glucose oxidation. In this work, we fabricated a two-dimensional cobalt-based zeolitic imidazolate framework (ZIF-L) as the electrode material for catalyzing glucose oxidation in alkaline conditions. Our explorations revealed that while the initial glucose catalytic response varied among ZIF-L samples with differing thicknesses, the ultimate steady-state catalytic performance remained largely consistent. This phenomenon arose from the transformation of ZIF-L with distinct thicknesses into CoOOH with uniform morphological and structural characteristics during the glucose catalysis process. And in situ Raman spectroscopy elucidated the sustained equilibrium within the glucose catalytic system, wherein the dynamic interconversion between CoOOH and Co(OH)2 governs the overall process. This study contributes to an enhanced understanding of the glucose catalytic mechanism aspects of nonenzymatic glucose sensor electrode materials, offering insights that serve as inspiration for the development of advanced glucose electrode materials.
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The design of catalysts has attracted a great deal of attention in the field of electrocatalysis. The accurate design of the catalysts can avoid an unnecessary process that occurs during the blind trial. Based on the interaction between different metal species, a metallic compound supported by the carbon nanotube was designed. Among these compounds, RhFeP2CX (R-RhFeP2CX-CNT) was found to be in a rich-electron environment at the Fermi level (denoted as a flat Fermi surface), beneficial to the hydrogen evolution reaction (HER). R-RhFeP2CX-CNT exhibits a small overpotential of 15 mV at the current density of 10 mA·cm-2 in acidic media. Moreover, the mass activity of R-RhFeP2CX-CNT is 21597 A·g-1, which also demonstrates the advance of the active sites on R-RhFeP2CX-CNT. Therefore, R-RhFeP2CX-CNT can be an alternative catalyst applied in practical production, and the strategies of a flat Fermi surface will be a reliable strategy for catalyst designing.
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Millimeter-wave and short-range wireless communication is an important part of the Internet of Things due to its advantages of high transmission speed and large data capacity. In this paper, two antenna arrays operating at typical millimeter-wave bands (45 and 60 GHz) based on graphene-assembled films (GAF) are proposed for short-range wireless communication application. The 45 GHz graphene-assembled film antenna array is in the form of a magnetoelectric dipole antenna with a strip slot coupling to achieve bidirectional radiation, which offers an operating bandwidth of 40-49.5 GHz with a realized gain of 11.8 dBi. The 60 GHz graphene-assembled film antenna utilizes a microstrip discontinuous radiation array to achieve radiation with an operating bandwidth of 59-64 GHz, reaching the peak realized gain of 14.92 dBi over the working frequency. Finally, we proposed an experimental validation to verify the transmission performance of both antenna arrays in an actual conference room. The results show that the signal drops slowly in the room with drop rates of 0.064 dB/cm (at 45 GHz) and 0.071 dB/cm (at 60 GHz), while it steeply dropped through the wall with the drop rates of 2.3 and 3.13 dB/cm, more than 35-fold difference in signal drop rates in the room and through the wall. It has been confirmed that the proposed antenna arrays can successfully realize fast indoor short-range wireless communication while also preventing signal leakage through walls, thereby enhancing the security of information. In summary, this is the first time that we have applied graphene-based materials to millimeter-wave and short-range wireless communications, revealing the significant potential of carbon-based materials in high-frequency communication systems.
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We present and numerically verify a functionally hybrid dual-mode tunable polarization conversion metasurface based on graphene and vanadium dioxide (VO2). The tunable polarization converter consists of two patterned graphene layers separated by grating which is composed of gold and VO2. Due to the existence of phase change material VO2, the polarization conversion mode can be switched flexibly between the transmission and reflection modes. Theoretical calculations show the proposed polarization conversion metasurface can obtain giant asymmetric transmission (AT) at 0.42 and 0.77 THz when VO2 is in the insulating state. Conversely, when VO2 is in the metallic state, the converter switches to the reflection mode, demonstrating broadband polarization conversion for both forward and backward incidences. Furthermore, the conductivity of graphene can be modulated by changing the gate voltage, which allows dynamic control polarization conversion bandwidth of the reflection mode as well as the AT of the transmission mode. The robustness of the metasurface has also been verified, the high polarization conversion efficiency and AT can be maintained over wide incidence angles up to 65° for both the xoz plane and yoz plane. These advantages make the proposed hybrid tunable polarization conversion metasurface a promising candidate for THz radiation switching and modulation.
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In this paper, a radio frequency identification (RFID) tag is designed and fabricated based on highly electrical and thermal conductive graphene films. The tag operates in the ultrahigh-frequency (UHF) band, which is suitable for high-power microwave environments of at least 800 W. We designed the protection structure to avoid charge accumulation at the antenna's critical positions. In the initial state, the read range of the anti-high-power microwave graphene film tag (AMGFT) is 10.43 m at 915 MHz. During the microwave heating experiment, the aluminum tag causes a visible electric spark phenomenon, which ablates the aluminum tag and its attachment, resulting in tag failure and serious safety issues. In contrast, the AMGFT is intact, with its entire read range curve growing and returning to its initial position as its temperature steadily decreases back to room temperature. In addition, the proposed dual-frequency tag further confirms the anti-high-power microwave performance of graphene film tags and provides a multi-scenario interactive application.
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With the ultimate atomic utilization, well-defined configuration of active sites and unique electronic properties, catalysts with single-atom sites (SASs) exhibit appealing performance for electrocatalytic green hydrogen generation from water splitting and further utilization via hydrogen-oxygen fuel cells, such that a vast majority of synthetic strategies toward SAS-based catalysts (SASCs) are exploited. In particular, room-temperature electrosynthesis under atmospheric pressure offers a novel, safe, and effective route to access SASs. Herein, the recent progress in ambient electrosynthesis toward SASs for electrocatalytic sustainable hydrogen generation and utilization, and future opportunities are discussed. A systematic summary is started on three kinds of ambient electrochemically synthetic routes for SASs, including electrochemical etching (ECE), direct electrodeposition (DED), and electrochemical leaching-redeposition (ELR), associated with advanced characterization techniques. Next, their electrocatalytic applications for hydrogen energy conversion including hydrogen evolution reaction, oxygen evolution reaction, overall water splitting, and oxygen reduction reaction are reviewed. Finally, a brief conclusion and remarks on future challenges regarding further development of ambient electrosynthesis of high-performance and cost-effective SASCs for many other electrocatalytic applications are presented.
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Since first developed, the conducting materials in wireless communication and electromagnetic interference (EMI) shielding devices have been primarily made of metal-based structures. Here, we present a graphene-assembled film (GAF) that can be used to replace copper in such practical electronics. The GAF-based antennas present strong anticorrosive behavior. The GAF ultra-wideband antenna covers the frequency range of 3.7 GHz to 67 GHz with the bandwidth (BW) of 63.3 GHz, which exceed ~110% than the copper foil-based antenna. The GAF Fifth Generation (5G) antenna array features a wider BW and lower sidelobe level compared with that of copper antennas. EMI shielding effectiveness (SE) of GAF also outperforms copper, reaching up to 127 dB in the frequency range of 2.6 GHz to 0.32 THz, with a SE per unit thickness of 6,966 dB/mm. We also confirm that GAF metamaterials exhibit promising frequency selection characteristics and angular stability as flexible frequency selective surfaces.
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Graphene and graphene-based materials gifted with high electrical conductivity are potential alternatives in various related fields. However, the electrical conductivity of the macro-graphene materials is much lower than their metal counterparts. Herein, we improved the electrical conductivity of reduced graphene oxide (rGO) based graphene assembled films (GAFs) by applying a series of compressive stress and systematically investigated the relationship between the compressive stress and the electrical conductivity. The result indicates that with increasing applied compressive stress, the sheet resistance increased as well, while the thickness decreased. Under the combined effect of these two competing factors, the number of charge carriers per unit volume increased dramatically, and the conductivity of compressed GAFs (c-GAFs) showed an initial increasing trend as we applied higher pressure and reached a maximum of 5.37 × 105 S/m at the optimal stress of 450 MPa with a subsequent decrease with stress at 550 MPa. Furthermore, the c-GAFs were fabricated into strain sensors and showed better stability and sensitivity compared with GAF-based sensors. This work revealed the mechanism of the tunable conductivity and presented a facile and universal method for improving the electrical conductivity of macro-graphene materials in a controllable manner and proved the potential applications of such materials in flexible electronics like antennas, sensors, and wearable devices.
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High-efficiency electromagnetic interference (EMI) shielding and heat dissipation synergy materials with flexible, robust, and environmental stability are urgently demanded in next-generation integration electronic devices. In this work, we report the lamellar MXene/Aramid nanofiber (ANF) composite films, which establish a nacre-like structure for EMI shielding and heat dissipation by using the intermittent filtration strategy. The MXene/ANF composite film filled with 50 wt % MXene demonstrates enhanced mechanical properties with a strength of 230.5 MPa, an elongation at break of 6.2%, and a toughness of 11.8 MJ·m3 (50 wt % MXene). These remarkable properties are attributed to the hydrogen bonding and highly oriented structure. Furthermore, due to the formation of the MXene conductive network, the MXene/ANF composite film shows an outstanding conductivity of 624.6 S/cm, an EMI shielding effectiveness (EMI SE) of 44.0 dB, and a superior specific SE value (SSE/t) of 18847.6 dB·cm2/g, which is better than the vacuum filtration film. Moreover, the MXene/ANF composite film also shows a great thermal conductivity of 0.43 W/m·K. The multifunctional MXene/ANF composite films with high-performance EMI shielding, heat dissipation, and joule heating show great potential in the field of aerospace, military, microelectronics, microcircuit, and smart wearable electronics.
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Assembling pristine graphene into freestanding films featuring high electrical conductivity, superior flexibility, and robust mechanical strength aims at meeting the all-around high criteria of new-generation electronics. However, voids and defects produced in the macroscopic assembly process of graphene nanosheets severely degrade the performance of graphene films, and mechanical brittleness often limits their applications in wide scenarios. To address such challenges, an electrostatic-repulsion aligning strategy is demonstrated to produce highly conductive, ultraflexible, and multifunctional graphene films. Typically, the high electronegativity of titania nanosheets (TiNS) induces the aligning of negatively charged graphene nanosheets via electrostatic repulsion in the film assembly. The resultant graphene films show fine microstructure, enhanced mechanical properties, and improved electrical conductivity up to 1.285 × 105 S m-1 . Moreover, the graphene films can withstand 5000 repeated folding without structural damage and electrical resistance fluctuation. These comprehensive improved properties, combined with the facile synthesis method and scalable production, make these graphene films a promising platform for electromagnetic interference (EMI) shielding and thermal-management applications in smart and wearable electronics.
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Numerous voids among the incompact layer-structure of MXene films result in their low ambient stability and poor innate conductivity for electromagnetic interference (EMI) shielding. Herein, we report a bridging-sheet-size-controlled densification process of MXene films by applying graphene oxide (GO) as a bridging agent. Specifically, the sheet size of GO is tailored to quantify a negative correlation of sheet size with densification for directing the preparation of most compact MXene-GO films. Benefiting from the shortest electron-transport-distance in the most compact structure, the conductivity of the MXene-GO film achieves 1.7 times (â¼1.6 × 105 S/m) that of MXene film. The EMI shielding performance (5.2 × 106 dB/m) reaches the record-value among reported MXene films at 10 µm-scale thickness. Moreover, the compact structure boosts the ambient stability of MXene-GO films where the conductivity and EMI shielding performance remain 88.7% and 90.0% after 15 days, respectively. The findings rationale the structure-activity relationship of compact MXene films for flexible electronics.
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Conventional techniques (e.g., culture-based method) for bacterial detection typically require a central laboratory and well-trained technicians, which may take several hours or days. However, recent developments within various disciplines of science and engineering have led to a major paradigm shift in how microorganisms can be detected. The analytical sensors which are widely used for medical applications in the literature are being extended for rapid and on-site monitoring of the bacterial pathogens in food, water and the environment. Especially, within the low-resource settings such as low and middle-income countries, due to the advantages of low cost, rapidness and potential for field-testing, their use is indispensable for sustainable development of the regions. Within this context, this paper discusses analytical methods and biosensors which can be used to ensure food safety, water quality and environmental monitoring. In brief, most of our discussion is focused on various rapid sensors including biosensors and microfluidic chips. The analytical performances such as the sensitivity, specificity and usability of these sensors, as well as a brief comparison with the conventional techniques for bacteria detection, form the core part of the discussion. Furthermore, we provide a holistic viewpoint on how future research should focus on exploring the synergy of different sensing technologies by developing an integrated multiplexed, sensitive and accurate sensors that will enable rapid detection for food safety, water and environmental monitoring.
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MXenes have exhibited potential for application in flexible devices owing to their remarkable electronic, optical, and mechanical properties. Printing strategies have emerged as a facile route for additive manufacturing of MXene-based devices, which relies on the rational design of functional inks with appropriate rheological properties. Herein, aqueous MXene/xanthan gum hybrid inks with tunable viscosity, excellent printability, and long-term stability are designed. Screen-printed flexible MXene films using such hybrid inks exhibit a high conductivity up to 4.8 × 104 S m-1 , which is suitable to construct multifunctional devices mainly including electromagnetic shielding, Joule heaters, and piezoresistive sensors. The average electromagnetic interference (EMI) shielding value can reach to 40.1 dB. In the Joule heater, the heating rate of printed MXene film can reach 20 °C s-1 under a driving voltage of 4 V, with a highest steady-state temperature of 130.8 °C. An MXene-based piezoresistive sensor prepared by the printing interdigital electrode also presents good sensing performance with a short response time of 130 ms and wide pressure region up to 30 kPa. As a result, screen-printed MXene film exhibits reinforced multifunctional performance, which is promising for application in the next-generation of intelligent and wearable devices.
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A macroscopic-assembled graphene oxide (GO) membrane with sustainable high strength presents a bright future for its applications in ionic and molecular filtration for water purification or fast force response for sensors. Traditionally, the bottom-up macroscopic assembly of GO sheets is optimized by widening the interlaminar space for expediting water passage, frequently leading to a compromise in strength, assembly time, and ensemble thickness. Herein, we rationalize this strategy by implanting a superhydrophilic bridge of cobalt-based metal-organic framework nanosheets (NMOF-Co) as an additional water "aisle" into the interlaminar space of GO sheets (GO/NMOF-Co), resulting in a high-strength macroscopic membrane ensemble with tunable thickness from the nanometer scale to the centimeter scale. The GO/NMOF-Co membrane assembly time is only 18 s, 30800 times faster than that of pure GO (154 h). More importantly, the obtained membrane attains a strength of 124.4 MPa, which is more than 3 times higher than that of the GO membrane prepared through filtration. The effect of hydrophilicity on membrane assembly is also investigated by introducing different intercalants, suggesting that, except for the interlamellar spacing, the interlayered hydrophilicity plays a more decisive role in the macroscopic assembly of GO membranes. Our results give a fundamental implication for fast macroscopic assembly of high-strength 2D materials.
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We explore the selective electrocatalytic hydrogenation of lignin monomers to methoxylated chemicals, of particular interest, when powered by renewable electricity. Prior studies, while advancing the field rapidly, have so far lacked the needed selectivity: when hydrogenating lignin-derived methoxylated monomers to methoxylated cyclohexanes, the desired methoxy group (-OCH3) has also been reduced. The ternary PtRhAu electrocatalysts developed herein selectively hydrogenate lignin monomers to methoxylated cyclohexanes-molecules with uses in pharmaceutics. Using X-ray absorption spectroscopy and in situ Raman spectroscopy, we find that Rh and Au modulate the electronic structure of Pt and that this modulating steers intermediate energetics on the electrocatalyst surface to facilitate the hydrogenation of lignin monomers and suppress C-OCH3 bond cleavage. As a result, PtRhAu electrocatalysts achieve a record 58% faradaic efficiency (FE) toward 2-methoxycyclohexanol from the lignin monomer guaiacol at 200 mA cm-2, representing a 1.9× advance in FE and a 4× increase in partial current density compared to the highest productivity prior reports. We demonstrate an integrated lignin biorefinery where wood-derived lignin monomers are selectively hydrogenated and funneled to methoxylated 2-methoxy-4-propylcyclohexanol using PtRhAu electrocatalysts. This work offers an opportunity for the sustainable electrocatalytic synthesis of methoxylated pharmaceuticals from renewable biomass.
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Flexible electronic devices are widely used in the Internet of Things, smart home and wearable devices, especially in carriers with irregular curved surfaces. Light weight, flexible and corrosion-resistant carbon-based materials have been extensively investigated in RF electronics. However, the insufficient electrical conductivity limits their further application. In this work, a flexible and low-profile dual-band Vivaldi antenna based on highly conductive graphene-assembled films (GAF) is proposed for 5G Wi-Fi applications. The proposed GAF antenna with the profile of 0.548 mm comprises a split ring resonator and open circuit half wavelength resonator to implement the dual band-notched characteristic. The operating frequency of the flexible GAF antenna covers the Wi-Fi 6e band, 2.4-2.45 GHz and 5.15-7.1 GHz. Different conformal applications are simulated by attaching the antenna to the surface of cylinders with different radii. The measured results show that the working frequency bands and the radiation patterns of the GAF antenna are relatively stable, with a bending angle of 180°. For demonstration of practical application, the GAF antennas are conformed to a commercial router. The spectral power of the GAF antenna router is greater than the copper antenna router, which means a higher signal-to-noise ratio and a longer transmission range can be achieved. All results indicate that the proposed GAF antenna has broad application prospects in next generation Wi-Fi.