Efficient Preconstruction of Three‑Dimensional Graphene Networks for Thermally Conductive Polymer Composites

Electronic devices generate heat during operation and require efficient thermal management to extend the lifetime and prevent performance degradation.Featured by its exceptional thermal conductivity,graphene is an ideal functional filler for fabricating thermally conductive polymer composites to provide efficient thermal management.Extensive studies have been focusing on constructing graphene networks in polymer composites to achieve high thermal conductivities.Compared with conventional composite fabrications by directly mixing graphene with polymers,preconstruction of three-dimensional graphene networks followed by backfilling polymers represents a promising way to produce composites with higher performances,enabling high manufacturing flexibility and controllability.In this review,we first summarize the factors that affect thermal conductivity of graphene composites and strategies for fabricating highly thermally conductive graphene/polymer composites.Subsequently,we give the reasoning behind using preconstructed three-dimensional graphene networks for fabricating thermally conductive polymer composites and highlight their potential applications.Finally,our insight into the existing bottlenecks and opportunities is provided for developing preconstructed porous architectures of graphene and their thermally conductive composites.

A green cross-linking method for the preparation of renewable threedimensional graphene sponges for efficient adsorption of Congo red dye

Graphene-based materials possess significant potential for the treatment of dye wastewater due to their exceptional adsorption properties toward stubborn pollutants.However,their utilization is hindered by high preparation costs,low yields,environmental pollution during synthesis,and challenges in regenerating the adsorbent.This study proposes a novel approach to address these limitations by developing nitrogen-doped three-dimensional(3D)polyvinyl alcohol(PVA)crosslinked graphene sponges(N-PGA)using a cross-linking method with ammonium carbonate.This method offers a relatively mild,environmentally friendly approach.Ammonium carbonate serves as both a reducing and modifying agent,facilitating the formation of the intrinsic structure of N-PGA and acting as a nitrogen source.Meanwhile,PVA is utilized as the cross-linking agent.The results demonstrate that N-PGA exhibits a favorable internal 3D hierarchical porous structure and possesses robust mechanical properties.The measured specific surface area(BET)of N-PGA was as high as406.538 m^(2)·g^(-1),which was favorable for its efficient adsorption of Congo red(CR)dye molecules.At an initial concentration of 50 mg·L^(-1),N-PGA achieved an impressive removal rate of 89.6%and an adsorption capacity of 112 mg·g^(-1)for CR dye.Furthermore,it retained 79%of its initial adsorption capacity after 10 cycles,demonstrating excellent regeneration performance.In summary,the synthesized N-PGA displays remarkable efficacy in the adsorption of CR dye in wastewater,opening up new possibilities for utilizing 3D porous graphene nanomaterials as efficient adsorbents in wastewater treatment.

Mixed‑Dimensional Assembly Strategy to Construct Reduced Graphene Oxide/Carbon Foams Heterostructures for Microwave Absorption,Anti‑Corrosion and Thermal Insulation

Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.

Spectral and Morphological Analysis of Graphene-Based Two- Dimensional Carbon Materials

This paper describes the spectral and morphological analysis of graphene, N-doped graphene, and graphenemodified with functional groups. The similarities and differences in the surface and microstructure are characterizedby infrared spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, andtransmission electron microscopy. Compared with high-purity graphene, the introduction of functional groups leads to moredefects in the two-dimensional structure. The quality of graphene, reflected by the intensity ratio of peak D and G modesin the Raman spectroscopy, is consistent with that observed by scanning electron microscopy and transmission electronmicroscopy. The infrared spectra of graphene-based two-dimensional carbon materials are different from that of high-puritygraphene, and the absorption peaks of the functional groups are obvious. The X-ray photoelectron spectroscopy resultsillustrate the diverse chemical states of carbon, and the atomic ratio of carbon to oxygen directly reflects the quality ofthe graphene-based materials. The results of electron microscopy and spectroscopic characterization of graphene samplesprovide an excellent basis for a wide range of applications in graphene production and quality control.

Three-Dimensional N-Doped Carbon Nanotube/Graphene Composite Aerogel Anode to Develop High-Power Microbial Fuel Cell

Optimizing the structure of electrode materials is one of the most effective strategies for designing high-power microbial fuel cells(MFCs).However,electrode materials currently suffer from a series of shortcomings that limit the output of MFCs,such as high intrinsic resistance,poor electrolyte wettability,and low microbial load capacity.Here,a three-dimensional(3D)nitrogen-doped multiwalled carbon nanotube/graphene(N-MWCNT/GA)composite aerogel is synthesized as the anode for MFCs.Comparing nitrogen-doped GA,MWCNT/GA,and N-MWCNT/GA,the macroporous hydrophilic N-MWCNT/GA electrode with an average pore size of 4.24μm enables high-density loading of the microbes and facilitates extracellular electron transfer with low intrinsic resistance.Consequently,the hydrophilic surface of N-MWCNT can generate high charge mobility,enabling a high-power output performance of the MFC.In consequence,the MFC system based on N-MWCNT/GA anode exhibits a peak power density and output voltage of 2977.8 mW m^(−2)and 0.654 V,which are 1.83 times and 16.3%higher than those obtained with MWCNT/GA,respectively.These results demonstrate that 3D N-MWCNT/GA anodes can be developed for high-power MFCs in different environments by optimizing their chemical and microstructures.

Green synthesis of three-dimensional magnesium ferrite/titanium dioxide/reduced graphene from Garcinia mangostana extract for crystal violet photodegradation and antibacterial activity

In this study,three-dimensional porous magnesium ferrite/titanium dioxide/reduced graphene oxide(Mg Fe_2O_(4)-GM/TiO_(2)/rGO(MGTG))was successfully synthesized via green and hydrothermal-supported co-precipitation methods using the extract of Garcinia mangostana(G.mangostana)as a reducing agent.The characterization results indicate the successful formation of the nano/micro Mg Fe_(2)O_(4)(MFO)and TiO_(2) on the structure of the reduced graphene oxide(rGO),which can also act as efficient support,alleviating the agglomeration of the nano/micro MFO and TiO_(2).The synergic effects of the adsorption and photodegradation activity of the material were investigated according to the removal of crystal violet(CV)under ultraviolet light.The effects of catalyst dosage,CV concentration,and p H on the CV removal efficiency of the MGTG were also investigated.According to the results,the CV photodegradation of the MGTG-200 corresponded to the pseudo-first-order kinetic model.The reusability of the material after 10 cycles also showed a removal efficiency of 92%.This happened because the materials can easily be recollected using external magnets.In addition,according to the effects of different free radicals·O_(2)^(-),h^(+),and·OH on the photodegradation process,the photocatalysis mechanism of the MGTG was also thoroughly suggested.The antibacterial efficiency of the MGTG was also evaluated according to the inhibition of the Gram-positive bacteria strain Staphylococcus aureus(S.aureus).Concurrently,the antibacterial mechanism of the fabricated material was also proposed.These results confirm that the prepared material can be potentially employed in a wide range of applications,including wastewater treatment and antibacterial activity.

Highly Thermoconductive,Strong Graphene‑Based Composite Films by Eliminating Nanosheets Wrinkles

Graphene-based thermally conductive composites have been proposed as effective thermal management materials for cooling high-power electronic devices.However,when flexible graphene nanosheets are assembled into macroscopic thermally conductive composites,capillary forces induce shrinkage of graphene nanosheets to form wrinkles during solution-based spontaneous drying,which greatly reduces the thermal conductivity of the composites.Herein,graphene nanosheets/aramid nanofiber(GNS/ANF)composite films with high thermal conductivity were prepared by in-plane stretching of GNS/ANF composite hydrogel networks with hydrogen bonds andπ-πinteractions.The in-plane mechanical stretching eliminates graphene nanosheets wrinkles by suppressing inward shrinkage due to capillary forces during drying and achieves a high in-plane orientation of graphene nanosheets,thereby creating a fast in-plane heat transfer channel.The composite films(GNS/ANF-60 wt%)with eliminated graphene nanosheets wrinkles showed a significant increase in thermal conductivity(146 W m^(−1)K^(−1))and tensile strength(207 MPa).The combination of these excellent properties enables the GNS/ANF composite films to be effectively used for cooling flexible LED chips and smartphones,showing promising applications in the thermal management of high-power electronic devices.

Three-dimensional MoS_2/reduced graphene oxide aerogel as a macroscopic visible-light photocatalyst

Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide（MoS2） is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide（MoS2/RGO） aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr（Ⅵ） in comparison with the MoS2 powder.In addition,the low density（56.1 mg/cm^3） of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.

Tracking Regulatory Mechanism of Trace Fe on Graphene Electromagnetic Wave Absorption

Polarization and conductance losses are the fundamental dielectric attenuation mechanisms for graphene-based absorbers, but it is not fully understood in revealing the loss mechanism of affect graphene itself. For the first time, the reduced graphene oxide(RGO) based absorbers are developed with regulatory absorption properties and the absorption mechanism of RGO is mainly originated from the carrier injection behavior of trace metal Fe nanosheets on graphene. Accordingly, the minimum reflection loss(RLmin) of Fe/RGO-2composite reaches-53.38 dB(2.45 mm), and the effective absorption bandwidth achieves 7.52 GHz(2.62 mm) with lower filling loading of 2 wt%. Using off-axis electron hologram testing combined with simulation calculation and carrier transport property experiments, we demonstrate here the carrier injection behavior from Fe to graphene at the interface and the induced charge accumulation and rearrangement, resulting in the increased interfacial and dipole polarization and the conductance loss. This work has confirmed that regulating the dielectric property of graphene itself by adding trace metals can not only ensure good impedance matching, but also fully exploit the dielectric loss ability of graphene at low filler content,which opens up an efficient way for designing lightweight absorbers and may be extended to other types materials.

Carbon nanocages bridged with graphene enable fast kinetics for dual-carbon lithium-ion capacitors

Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.

Greatly enhanced corrosion/wear resistances of epoxy coating for Mg alloy through a synergistic effect between functionalized graphene and insulated blocking layer

The poor corrosion and wear resistances of Mg alloys seriously limit their potential applications in various industries.The conventional epoxy coating easily forms many intrinsic defects during the solidification process,which cannot provide sufficient protection.In the current study,we design a double-layer epoxy composite coating on Mg alloy with enhanced anti-corrosion/wear properties,via the spin-assisted assembly technique.The outer layer is functionalized graphene(FG)in waterborne epoxy resin(WEP)and the inner layer is Ce-based conversion(Ce)film.The FG sheets can be homogeneously dispersed within the epoxy matrix to fill the intrinsic defects and improve the barrier capability.The Ce film connects the outer layer with the substrate,showing the transition effect.The corrosion rate of Ce/WEP/FG composite coating is 2131 times lower than that of bare Mg alloy,and the wear rate is decreased by~90%.The improved corrosion resistance is attributed to the labyrinth effect(hindering the penetration of corrosive medium)and the obstruction of galvanic coupling behavior.The synergistic effect derived from the FG sheet and blocking layer exhibits great potential in realizing the improvement of multi-functional integration,which will open up a new avenue for the development of novel composite protection coatings of Mg alloys.

N-doped graphene quantum dot-decorated N-TiO2/P-doped porous hollow g-C_(3)N_(4) nanotube composite photocatalysts for antibiotic photodegradation and H2 production

Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.

Radiative Blood-Based Hybrid Copper-Graphene Nanoliquid Flows along a Source-Heated Leaning Cylinder

Variant graphene,graphene oxides(GO),and graphene nanoplatelets(GNP)dispersed in blood-based copper(Cu)nanoliquids over a leaning permeable cylinder are the focus of this study.These forms of graphene are highly beneficial in the biological and medical fields for cancer therapy,anti-infection measures,and drug delivery.The non-Newtonian Sutterby(blood-based)hybrid nanoliquid flows are generalized within the context of the Tiwari-Das model to simulate the effects of radiation and heating sources.The governing partial differential equations are reformulated into a nonlinear set of ordinary differential equations using similar transformational expressions.These equations are then transformed into boundary value problems through a shooting technique,followed by the implementation of the bvp4c tool in MATLAB.The influences of various parameters on the model’s nondimensional velocity and temperature profiles,reduced skin friction,and reduced Nusselt number are presented for detailed discussions.The results indicated that Cu-GNP/blood and Cu-GO/blood hybrid nanofluids exhibit the lowest and highest velocity distributions,respectively,for increased nanoparticles volume fraction,curvature parameter,Sutterby fluid parameter,Hartmann number,and wall permeability parameter.Conversely,opposite trends are observed for the temperature distribution for all considered parameters,except the mixed convection parameter.Increases in the reduced skin friction magnitude and the reduced Nusselt number with higher values of graphene/GO/GNP nanoparticle volume fraction are also reported.Finally,GNP is identified as the superior heat conductor,with an average increase of approximately 5%and a peak of 7.8%in the reduced Nusselt number compared to graphene and GO nanoparticles in the Cu/blood nanofluids.

Aggregation-regulated bioreduction process of graphene oxide by Shewanella bacteria

The bioreduction of graphene oxide(GO)using environmentally functional bacteria such as Shewanella represents a green approach to produce reduced graphene oxide(rGO).This process differs from the chemical reduction that involves instantaneous molecular reactions.In bioreduction,the contact of bacterial cells and GO is considered the rate-limiting step.To reveal how the bacteria-GO integration regulates rGO production,the comparative experiments of GO and three Shewanella strains were carried out.Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,Raman spectroscopy,and atomic force microscopy were used to characterize the reduction degree and the aggregation degree.The results showed that a spontaneous aggregation of GO and Shewanella into the condensed entity occurred within 36 h.A positive linear correlation was established,linking three indexes of the aggregation potential,the bacterial reduction ability,and the reduction degree(ID/IG)comprehensively.

对二维Graphene/VS_(2)/BN范德华多层异质结构作为LIBs的阳极材料的相关研究

通过范德华尔斯作用将单层石墨烯(Graphene)、单层二硫化钒(VS2)和单层氮化硼(BN)构建成Graphene/VS2/BN范德华三层异质结构,并将其与不同数量的锂结合,研究了其作为锂离子电池(Li-Ion Batterys,LIBs)中阳极电极材料的可行性.Graphene/VS_(2)/BN范德华三层异质结构具有-0.33 e V/A2的形成能,具有较强的稳定性,理论上可实现合成.同时,计算了Graphene/VS_(2)/BN范德华异质结构的平面内刚度,得出的杨氏模量(Y)为886.88 N/m,高于单层VS_(2)的Y(82.5 N/m),具有较好的力学性能.Graphene/VS_(2)/BN范德华三层异质结构表面和界面上吸附Li的吸附能(-5~-2 e V)远大于相应单层的吸附能,表明其对Li具有较好的吸附性能.Li在Graphene/VS_(2)/BN范德华三层异质结构的不同表面和界面处迁移时的扩散势垒非常小(0.3~0.6 e V),对电池速率性能极为有利.Graphene/VS_(2)/BN范德华三层异质结构在LIBs的阳极电极材料方面的应用具有广泛的前景.

Valley-dependent transport in a mescoscopic twisted bilayer graphene device

We study the valley-dependent electron transport in a four-terminal mesoscopic device of the two monolayer graphene nanoribbons vertically stacked together, where the intersection forms a bilayer graphene lattice with a controllable twist angle. Using a tight-binding lattice model, we show that the longitudinal and transverse conductances exhibit significant valley polarization in the low energy regime for small twist angles. As the twist angle increases, the valley polarization shifts to the high energy regime. This arises from the regrouping effect of the electron band in the twisted bilayer graphene region. But for relatively large twist angles, no significant valley polarization is observed. These results are consistent with the spectral densities of the twisted bilayer graphene.

Highly efficient three-dimensional solar evaporator for zero liquid discharge desalination of high-salinity brine

Solar-driven interfacial evaporation is a promising technology for freshwater production from seawater,but salt accumulation on the evaporator surface hinders its performance and sustainability.In this study,we report a simple and green strategy to fabricate a three-dimensional porous graphene spiral roll(3GSR)that enables highly efficient solar evaporation,salt collection,and water production from near-saturated brine with zero liquid discharge(ZLD).The 3GSR design facilitates energy recovery,radial brine transport,and directional salt crystallization,thereby resulting in an ultrahigh evaporation rate of 9.05 kg m^(-2) h^(-1)6 in 25 wt%brine under 1-sun illumina-tion for 48 h continuously.Remarkably,the directional salt crystallization on its outer surface not only enlarges the evaporation area but also achieves an ultrahigh salt collection rate of 2.92 kg m^(-2) h^(-1),thus enabling ZLD desalination.Additionally,3GSR exhibits a record-high water production rate of 3.14 kg m^(-2) h^(-1) in an outdoor test.This innovative solution offers a highly efficient and continuous solar desalination method for water production and ZLD brine treatment,which has great implications for addressing global water scarcity and environmental issues arising from brine disposal.

In vitro investigations on the effects of graphene and graphene oxide on polycaprolactone bone tissue engineering scaffolds

Polycaprolactone(PCL)scaffolds that are produced through additive manufacturing are one of the most researched bone tissue engineering structures in the field.Due to the intrinsic limitations of PCL,carbon nanomaterials are often investigated to reinforce the PCL scaffolds.Despite several studies that have been conducted on carbon nanomaterials,such as graphene(G)and graphene oxide(GO),certain challenges remain in terms of the precise design of the biological and nonbiological properties of the scaffolds.This paper addresses this limitation by investigating both the nonbiological(element composition,surface,degradation,and thermal and mechanical properties)and biological characteristics of carbon nanomaterial-reinforced PCL scaffolds for bone tissue engineering applications.Results showed that the incorporation of G and GO increased surface properties(reduced modulus and wettability),material crystallinity,crystallization temperature,and degradation rate.However,the variations in compressive modulus,strength,surface hardness,and cell metabolic activity strongly depended on the type of reinforcement.Finally,a series of phenomenological models were developed based on experimental results to describe the variations of scaffold’s weight,fiber diameter,porosity,and mechanical properties as functions of degradation time and carbon nanomaterial concentrations.The results presented in this paper enable the design of three-dimensional(3D)bone scaffolds with tuned properties by adjusting the type and concentration of different functional fillers.

Improving the operational stability of perovskite solar cells with cesium-doped graphene oxide interlayer

Perovskite solar cells(PSCs)have made great advances in terms of power conversion efficiency(PCE),yet their subpar stability continues to hinder their commercialization.The interface between the perovskite layer and the charge-carrier transporting layers plays a crucial role in undermining the stability of PSCs.In this work,we propose a strategy to stabilize high-performance PSCs with PCE over 23%by introducing a cesium-doped graphene oxide(GO-Cs)as an interlayer between the perovskite and hole-transporting material.The GO-Cs treated PSCs exhibit excellent operational stability with a projected T80(the time where the device PCE reduces to 80%of its initial value)of 2143 h of operation at the maximum powering point under one sun illumination.

Use of the epitaxial MTBs as a 1D gate(Lg=0.4 nm)for the construction of scaling down two-dimensional field-effect transistors

In recent years,there has been a significant increase in research focused on the growth of large-area single crystals.Rajan et al.[1]recently achieved the growth of large-area monolayers of transition-metal chalcogenides through assisted nucleation.The quality of molecular beam epitaxy(MBE)-grown two-dimensional(2D)materials can be greatly enhanced by using sacrificial species deposited simultaneously from an electron beam evaporator during the growth process.This technique notably boosts the nucleation rate of the target epitaxial layer,resulting in large,homogeneous monolayers with improved quasiparticle lifetimes and fostering the development of epitaxial van der Waals heterostructures.Additionally,micrometer-sized silver films have been formed at the air-water interface by directly depositing electrospray-generated silver ions onto an aqueous dispersion of reduced graphene oxide under ambient conditions[2].