Highly Aligned Graphene Aerogels for Multifunctional Composites

Stemming from the unique in-plane honeycomb lattice structure and the sp^(2)hybridized carbon atoms bonded by exceptionally strong carbon–carbon bonds,graphene exhibits remarkable anisotropic electrical,mechanical,and thermal properties.To maximize the utilization of graphene’s in-plane properties,pre-constructed and aligned structures,such as oriented aerogels,films,and fibers,have been designed.The unique combination of aligned structure,high surface area,excellent electrical conductivity,mechanical stability,thermal conductivity,and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions,enabling advancements in diverse fields.This review provides a comprehensive overview of recent advances in highly aligned graphene aerogels and their composites.It highlights the fabrication methods of aligned graphene aerogels and the optimization of alignment which can be estimated both qualitatively and quantitatively.The oriented scaffolds endow graphene aerogels and their composites with anisotropic properties,showing enhanced electrical,mechanical,and thermal properties along the alignment at the sacrifice of the perpendicular direction.This review showcases remarkable properties and applications of aligned graphene aerogels and their composites,such as their suitability for electronics,environmental applications,thermal management,and energy storage.Challenges and potential opportunities are proposed to offer new insights into prospects of this material.

Tuning the surface electronic structure of noble metal aerogels to promote the electrocatalytic oxygen reduction

The sluggish kinetics of the oxygen reduction reaction(ORR)is the bottleneck for various electrochemical energy conversion devices.Regulating the electronic structure of electrocatalysts by ligands has received particular attention in deriving valid ORR electrocatalysts.Here,the surface electronic structure of Ptbased noble metal aerogels(NMAs)was modulated by various organic ligands,among which the electron-withdrawing ligand of 4-methylphenylene effectively boosted the ORR electrocatalysis.Theoretical calculations suggested the smaller energy barrier for the transformation of O^(*) to OH^(*) and downshift the d-band center of Pt due to the interaction between 4-methylphenylene and the surface metals,thus enhancing the ORR intrinsic activity.Both Pt3Ni and Pt Pd aerogels with 4-methylphenylene decoration performed significant enhancement in ORR activity and durability in different media.Remarkably,the 4-methylphenylene modified Pt Pd aerogel exhibited the higher halfwave potential of 0.952 V and the mass activity of 10.2 times of commercial Pt/C.This work explained the effect of electronic structure on ORR electrocatalytic properties and would promote functionalized NMAs as efficient ORR electrocatalysts.

Harness High-Temperature Thermal Energy via Elastic Thermoelectric Aerogels

Despite notable progress in thermoelectric(TE)materials and devices,developing TE aerogels with high-temperature resistance,superior TE performance and excellent elasticity to enable self-powered high-temperature monitoring/warning in industrial and wearable applications remains a great challenge.Herein,a highly elastic,flame-retardant and high-temperature-resistant TE aerogel,made of poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate)/single-walled carbon nanotube(PEDOT:PSS/SWCNT)composites,has been fabricated,displaying attractive compression-induced power factor enhancement.The as-fabricated sensors with the aerogel can achieve accurately pressure stimuli detection and wide temperature range monitoring.Subsequently,a flexible TE generator is assembled,consisting of 25 aerogels connected in series,capable of delivering a maximum output power of 400μW when subjected to a temperature difference of 300 K.This demonstrates its outstanding high-temperature heat harvesting capability and promising application prospects for real-time temperature monitoring on industrial high-temperature pipelines.Moreover,the designed self-powered wearable sensing glove can realize precise wide-range temperature detection,high-temperature warning and accurate recognition of human hand gestures.The aerogel-based intelligent wearable sensing system developed for firefighters demonstrates the desired self-powered and highly sensitive high-temperature fire warning capability.Benefitting from these desirable properties,the elastic and high-temperature-resistant aerogels present various promising applications including self-powered high-temperature monitoring,industrial overheat warning,waste heat energy recycling and even wearable healthcare.

Highly Porous Yet Transparent Mechanically Flexible Aerogels Realizing Solar-Thermal Regulatory Cooling

The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.

Three-dimensional porous bimetallic metal–organic framework/gelatin aerogels: A readily recyclable peroxymonosulfate activator for efficient and continuous organic dye removal

As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.

In Situ Mineralization of Biomass-Derived Hydrogels Boosts Capacitive Electrochemical Energy Storage in Free-Standing 3D Carbon Aerogels

Here,a novel fabrication method for making free-standing 3D hierarchical porous carbon aerogels from molecularly engineered biomass-derived hydrogels is presented.In situ formed flower-like CaCO_(3)molecularly embedded within the hydrogel network regulated the pore structure during in situ mineralization assisted one-step activation graphitization(iMAG),while the intrinsic structural integrity of the carbon aerogels was maintained.The homogenously distributed minerals simultaneously acted as a hard template,activating agent,and graphitization catalyst.The decomposition of the homogenously distributed CaCO_(3)during iMAG followed by the etching of residual CaO through a mild acid washing endowed a robust carbon aerogel with high porosity and excellent electrochemical performance.At 0.5 mA cm^(-2),the gravimetric capacitance increased from 0.01 F g^(-1)without mineralization to 322 F g^(-1)with iMAG,which exceeds values reported for any other free-standing or powder-based biomass-derived carbon electrodes.An outstanding cycling stability of~104%after 1000 cycles in 1 M HClO4 was demonstrated.The assembled symmetric supercapacitor device delivered a high specific capacitance of 376 F g^(-1)and a high energy density of 26 W h kg^(-1)at a power density of 4000 W kg^(-1),with excellent cycling performance(98.5%retention after 2000 cycles).In combination with the proposed 3D printed mold-assisted solution casting(3DMASC),iMAG allows for the generation of free-standing carbon aerogel architectures with arbitrary shapes.Furthermore,the novel method introduces flexibility in constructing free-standing carbon aerogels from any ionically cross-linkable biopolymer while maintaining the ability to tailor the design,dimensions,and pore size distribution for specific energy storage applications.

Synthesis and microwave absorption performance of heat-treated RF/SiO_(2)aerogels

The well-designed composite with satisfactory electromagnetic microwave absorption at high temperatures remains a serious challenge.Herein,we fabricated a resorcinol-formaldehyde/silica dioxide composite aerogel(RF/SiO_(2))with a three-dimensional network structure using sol-gel,atmospheric pressure drying technique as well as heat-treated processes to achieve enhanced microwave absorption capabilities in the low frequency range.The pristine RF/SiO_(2)aerogel presented a typical micropores structure with a surface area,porous volume,and density of 146.82 m^(2)/g,62.40%,and 0.28 cm^(3)/g,respectively.Remarkably,the RF/SiO_(2)aerogel showed an effective absorption bandwidth of 3.56 GHz and a minimum reflection loss value of-46.10 d B at 2.25 mm after being heat-treated at 1500°C,while the maximum effective absorption bandwidth was 3.60 GHz at 2.30 mm.The intricate three-dimensional networks possessed remarkable impedance matching,multiple attenuation mechanisms,interfacial polarization,and dielectric loss,which were attributed to the exceptional ability to absorb electromagnetic microwaves.It offered a fresh approach to creating adaptable and effective microwave absorption materials in military defense.

Theoretical study on the effective thermal conductivity of silica aerogels based on a cross-aligned and cubic pore model

Aerogel nanoporous materials possess high porosity, high specific surface area, and extremely low density due to their unique nanoscale network structure. Moreover, their effective thermal conductivity is very low, making them a new type of lightweight and highly efficient nanoscale super-insulating material. However, prediction of their effective thermal conductivity is challenging due to their uneven pore size distribution. To investigate the internal heat transfer mechanism of aerogel nanoporous materials, this study constructed a cross-aligned and cubic pore model(CACPM) based on the actual pore arrangement of SiO_(2) aerogel. Based on the established CACPM, the effective thermal conductivity expression for the aerogel was derived by simultaneously considering gas-phase heat conduction, solid-phase heat conduction, and radiative heat transfer. The derived expression was then compared with available experimental data and the Wei structure model. The results indicate that, according to the model established in this study for the derived thermal conductivity formula of silica aerogel, for powdery silica aerogel under the conditions of T = 298 K, a_(2)= 0.85, D_(1)= 90 μm, ρ = 128 kg/m^(3), within the pressure range of 0–10^(5)Pa, the average deviation between the calculated values and experimental values is 10.51%. In the pressure range of 10^(3)–10^(4)Pa, the deviation between calculated values and experimental values is within 4%. Under these conditions, the model has certain reference value in engineering verification. This study also makes a certain contribution to the research of aerogel thermal conductivity heat transfer models and calculation formulae.

Nanocellulose-Assisted Construction of Multifunctional MXene-Based Aerogels with Engineering Biomimetic Texture for Pressure Sensor and Compressible Electrode

Multifunctional architecture with intriguing structural design is highly desired for realizing the promising performances in wearable sensors and flexible energy storage devices.Cellulose nanofiber(CNF)is employed for assisting in building conductive,hyperelastic,and ultralight Ti_(3)C_(2)T_(x)MXene hybrid aerogels with oriented tracheid-like texture.The biomimetic hybrid aerogels are constructed by a facile bidirectional freezing strategy with CNF,carbon nanotube(CNT),and MXene based on synergistic electrostatic interaction and hydrogen bonding.Entangled CNF and CNT“mortars”bonded with MXene“bricks”of the tracheid structure produce good interfacial binding,and superior mechanical strength(up to 80%compressibility and extraordinary fatigue resistance of 1000 cycles at 50%strain).Benefiting from the biomimetic texture,CNF/CNT/MXene aerogel shows ultralow density of 7.48 mg cm^(-3)and excellent electrical conductivity(~2400 S m^(-1)).Used as pressure sensors,such aerogels exhibit appealing sensitivity performance with the linear sensitivity up to 817.3 kPa^(-1),which affords their application in monitoring body surface information and detecting human motion.Furthermore,the aerogels can also act as electrode materials of compressive solid-state supercapacitors that reveal satisfactory electrochemical performance(849.2 mF cm^(-2)at 0.8 mA cm^(-2))and superior long cycle compression performance(88%after 10,000 cycles at a compressive strain of 30%).

Fibrous MXene Aerogels with Tunable Pore of Contaminated Seawater

The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actual,oil-contaminated seawater remains a critical challenge,because the transport channels and evaporation interfaces of the current solar evaporators are easily blocked by the oil slicks,resulting in undermined evaporation rate and conversion efficiency.Herein,we propose a facile strategy for fabricating a modularized solar evaporator based on flexible MXene aerogels with arbitrarily tunable,highly ordered cellular/lamellar pore structures for high-efficiency oil interception and desalination.The core design is the creation of 1D fibrous MXenes with sufficiently large aspect ratios,whose superior flexibility and plentiful link forms lay the basis for controllable 3D assembly into more complicated pore structures.The cellular pore structure is responsible for effective contaminants rejection due to the multi-sieving effect achieved by the omnipresent,isotropic wall apertures together with underwater superhydrophobicity,while the lamellar pore structure is favorable for rapid evaporation due to the presence of continuous,large-area evaporation channels.The modularized solar evaporator delivers the best evaporation rate(1.48 kg m-2h-1)and conversion efficiency(92.08%)among all MXene-based desalination materials on oil-contaminated seawater.

Biomass Homogeneity Reinforced Carbon Aerogels Derived Functional Phase-Change Materials for Solar–Thermal Energy Conversion and Storage

We deviseda functional form stable compositephase-change materials(PCMs)toachieve a three-dimensional(3D)interconnectedporous carbon aerogel structure for encapsulating polyethyleneglycol(PEG).Anovelhomogeneity reinforced carbonaerogel witha well-interconnected porous structure was constructed bycombining a flexible carbonresource from biomass guar gum with hard-brittle carbonfrom polyimide,to overcome severeshrinkage andpoor mechanical performance of traditionalcarbon aerogel.Thesupportingcarbon aerogel-encapsulated PEG produced thenovel composite PCMswithgood structure stability andcomprehensive energy storage performance.Theresults showed thatthecomposite PCMsdisplayed awell-defined 3Dinterconnected structure,and theirenergy storage capacities were 171.5 and169.5 J/g,which changed onlyslightlyafter 100 thermalcycles,andthe compositescould maintainthe equilibrium temperature at50.0−58.1℃ for about 760.3 s.The thermal conductivityofthe compositescould reach0.62 W m^(−1) K^(−1),which effectively enhanced the thermalresponse rate.And thecomposite PCMs exhibited good leakage-proof performance andexcellent light–thermal conversion.The compressive strengthof thecomposite PCMscan improveupto 1.602 MPa.Results indicatethatthisstrategy canbe efficiently usedtodevelop novel composite PCMswithimproved comprehensive thermalperformance and high light–thermal conversion.

Modulating Pd e_(g) orbital occupancy in Pd-Au metallic aerogels for efficient carbon dioxide reduction

The electronic structure of electrocatalysts plays a critical role in energy conversion,whereas for an efficient catalyst,it is challenging to modulate the orbitals.Herein,we present a new strategy to modulate the e_(g) orbital occupancy of Pd by constructing composition-controllable Pd-Au metallic aerogels(MAs),optimizing the d-band center of Pd to achieve excellent performance for electrochemical carbon dioxide reduction reaction(CO_(2)RR).Specifically,Pd_(1)Au_(2) MAs achieve almost 100% Faraday efficiency(FE) of CO in the range of-0.40 to-0.80 V vs.reversible hydrogen electrode(RHE),as well as the long-term stability,being one of the best Pd-based materials for CO_(2)RR.The X-ray photoelectron spectroscopy(XPS) results and density functional theory(DFT) calculations demonstrate that the introduction of Au modulates the Pd e_(g) orbital occupancy,which significantly weakens *CO adsorption on Pd,reduces the CO_(2)RR energy barrier and consequently improves the electrocatalytic activity and stability for long-term applications.Our work highlights a new strategy for designing efficient electrocatalysts for CO_(2)RR and beyond.

Multifunctional MXene/C Aerogels for Enhanced Microwave Absorption and Thermal Insulation

Two-dimensional transition metal carbides and nitrides(MXene)have emerged as promising candidates for microwave absorption(MA)materials.However,they also have some drawbacks,such as poor impedance matching,high self-stacking tendency,and high density.To tackle these challenges,MXene nanosheets were incorporated into polyacrylonitrile(PAN)nanofibers and subsequently assembled into a three-dimensional(3D)network structure through PAN carbonization,yielding MXene/C aerogels.The 3D network effectively extends the path of microcurrent transmission,leading to enhanced conductive loss of electromagnetic(EM)waves.Moreover,the aerogel’s rich pore structure significantly improves the impedance matching while effectively reducing the density of the MXenebased absorbers.EM parameter analysis shows that the MXene/C aerogels exhibit a minimum reflection loss(RL_(min))value of−53.02 dB(f=4.44 GHz,t=3.8 mm),and an effective absorption bandwidth(EAB)of 5.3 GHz(t=2.4 mm,7.44–12.72 GHz).Radar cross-sectional(RCS)simulations were employed to assess the radar stealth effect of the aerogels,revealing that the maximum RCS reduction value of the perfect electric conductor covered by the MXene/C aerogel reaches 12.02 dB m^(2).In addition to the MA performance,the MXene/C aerogel also demonstrates good thermal insulation performance,and a 5-mm-thick aerogel can generate a temperature gradient of over 30℃ at 82℃.This study provides a feasible design approach for creating lightweight,efficient,and multifunctional MXene-based MA materials.

Fibrous Aerogels with Tunable Superwettability for High-Performance Solar-Driven Interfacial Evaporation

Solar-driven interfacial evaporation is an emerging technology for water desalination.Generally,double-layered structure with separate surface wettability properties is usually employed for evaporator construction.However,creating materials with tunable properties is a great challenge because the wettability of existing materials is usually monotonous.Herein,we report vinyltrimethoxysilane as a single molecular unit to hybrid with bacterial cellulose(BC)fibrous network,which can be built into robust aerogel with entirely distinct wettability through controlling assembly pathways.Siloxane groups or carbon atoms are exposed on the surface of BC nanofibers,resulting in either superhydrophilic or superhydrophobic aerogels.With this special property,single component-modified aerogels could be integrated into a double-layered evaporator for water desalination.Under 1 sun,our evaporator achieves high water evaporation rates of 1.91 and 4.20 kg m^(-2)h^(-1)under laboratory and outdoor solar conditions,respectively.Moreover,this aerogel evaporator shows unprecedented lightweight,structural robustness,long-term stability under extreme conditions,and excellent salt-resistance,highlighting the advantages in synthesis of aerogel materials from the single molecular unit.

Reconstruction and functionalization of aerogels by controlling mesoscopic nucleation to greatly enhance macroscopic performance

This work presents a strategy for the mesoscopic engineering of hierarchically structured sodium alginate(SA)aerogels to enhance the macroscopic performance.The strategy was implemented by meso-functionalizing and reorganizing SA aerogels via controlled heterogeneous nucleation,in which microcrystalline cellulose-manganese dioxide(MCC-MnO_(2))nano-crystallites worked as template.Due to the short rod-like structure and abundant hydroxyl groups of MCC-MnO_(2),the organized mesostructure of SA aerogels was reconstructed during the assembly of SA molecule chains,which gave rise to a significant enhancement in macroscopic performance of SA areogels.For instance,the functionalized and reconstructed MCC-MnO_(2)/SA aerogels acquired a more than 70%increase in mechanical strength with an excellent deformation recovery.Furthermore,an almost double enhancement of removal capacity for metal ions(i.e.,Cu^(2+)and Pb^(2+))and organic dyes(i.e.,congo red and methylene blue)was obtained for MnO_(2)/SA aerogels,with an 87%repossession of the pollutants removal performance after 5 operation cycles.

Controllable fabrication of carbon aerogels

Nano-pore carbon aerogels were prepared by the sol-gel polymerization of resorcinol (1,3-dihydroxybenzene)(C6H4(OH)2) with formaldehyde (HCHO) in a slightly basic aqueous solution, followed by super-critical drying under liquid carbon dioxide as super-critical media and carbonization at 700 ℃ under N2 gas atmosphere. The key of the work is to fabricate carbon aerogels with controllable nano-pore structure, which means extremely high surface area and sharp pore size distribution. Aiming to investigate the effects of preparation conditions on the gelation process, the bulk density, and the physical and chemical structure of the resultant carbon aerogels, the molar ratio of R/C (resorcinol to catalyst) and the amount of distilled water were varied, consequently two different sets of samples, with series of R/C ratio and RF/W (Resorcinol-Formaldehyde to water, or the content of reactant) ratio, were prepared. The result of N2 adsorption/desorption experiment at 77 K shows that the pore sizes decreasing from 11.4 down to 2.2 nm with the increasing of the molar ratio of R/C from 100 to 400, and/or, the pore sizes decreasing from 3.8 down to 1.6 nm with the increasing of reactant content from 0.4 to 0.6.

Photocatalytic activity of TiO_2 supported SiO_2-Al_2O_3 aerogels prepared from industrial fly ash

A ternary composite of TiO2 and a SiO2-Al2O3 aerogel with good photocatalytic activity was prepared by a simple sol-gel method with TiO2 nanoparticles and SiO2-Al2O3 aerogels derived from industrial fly ash.The structural features of the TiO2/SiO2-Al2O3 aerogel composite were investigated by X-ray powder diffraction,Fourier transform infrared spectroscopy,transmission electron microscopy,gas adsorption measurements and diffuse reflectance UV-visible spectroscopy.The optimal conditions for photocatalytic degradation of 2-sec-butyl-4,6-dinitrophenol（DNBP],included an initial DNBP concentration of 0.167 mmol/L at pH = 4.86 with a catalyst concentration of 6 g/L,under visible light irradiation for 5 h.A plausible mechanism is proposed for the photocatalytic degradation of DNBP.Our composite showed higher photocatalytic activity for DNBP degradation than that of pure TiO2.This indicates that this material can serve as an efficient photocatalyst for degradation of hazardous organic pollutants in wastewater.

Structural Engineering of Hierarchical Aerogels Comprised of Multi-dimensional Gradient Carbon Nanoarchitectures for Highly Efficient Microwave Absorption

Recently,multilevel structural carbon aerogels are deemed as attractive candidates for microwave absorbing materials.Nevertheless,excessive stack and agglomeration for low-dimension carbon nanomaterials inducing impedance mismatch are significant challenges.Herein,the delicate“3D helix-2D sheet-1D fiber-0D dot”hierarchical aerogels have been successfully synthesized,for the first time,by sequential processes of hydrothermal self-assembly and in-situ chemical vapor deposition method.Particularly,the graphene sheets are uniformly intercalated by 3D helical carbon nanocoils,which give a feasible solution to the mentioned problem and endows the as-obtained aerogel with abundant porous structures and better dielectric properties.Moreover,by adjusting the content of 0D core-shell structured particles and the parameters for growth of the 1D carbon nanofibers,tunable electromagnetic properties and excellent impedance matching are achieved,which plays a vital role in the microwave absorption performance.As expected,the optimized aerogels harvest excellent performance,including broad effective bandwidth and strong reflection loss at low filling ratio and thin thickness.This work gives valuable guidance and inspiration for the design of hierarchical materials comprised of dimensional gradient structures,which holds great application potential for electromagnetic wave attenuation.

3D Lamellar-Structured Graphene Aerogels for Thermal Interface Composites with High Through-Plane Thermal Conductivity and Fracture Toughness

Although thermally conductive graphene sheets are efficient in enhancing in-plane thermal conductivities of polymers,the resulting nanocomposites usually exhibit low through-plane thermal conductivities,limiting their application as thermal interface materials.Herein,lamellarstructured polyamic acid salt/graphene oxide(PAAS/GO)hybrid aerogels are constructed by bidirectional freezing of PAAS/GO suspension followed by lyophilization.Subsequently,PAAS monomers are polymerized to polyimide(PI),while GO is converted to thermally reduced graphene oxide(RGO)during thermal annealing at 300℃.Final graphitization at 2800℃ converts PI to graphitized carbon with the inductive effect of RGO,and simultaneously,RGO is thermally reduced and healed to high-quality graphene.Consequently,lamellar-structured graphene aerogels with superior through-plane thermal conduction capacity are fabricated for the first time,and its superior through-plane thermal conduction capacity results from its vertically aligned and closely stacked high-quality graphene lamellae.After vacuum-assisted impregnation with epoxy,the resultant epoxy composite with 2.30 vol% of graphene exhibits an outstanding through-plane thermal conductivity of as high as 20.0 W m^−1 K^−1,100 times of that of epoxy,with a record-high specific thermal conductivity enhancement of 4310%.Furthermore,the lamellar-structured graphene aerogel endows epoxy with a high fracture toughness,~1.71 times of that of epoxy.

Ultralight Magnetic and Dielectric Aerogels Achieved by Metal-Organic Framework Initiated Gelation of Graphene Oxide for Enhanced Microwave Absorption

The development of a convenient methodology for synthesizing the hierarchically porous aerogels comprising metal–organic frameworks(MOFs)and graphene oxide(GO)building blocks that exhibit an ultralow density and uniformly distributed MOFs on GO sheets is important for various applications.Herein,we report a facile route for synthesizing MOF/reduced GO(rGO)aerogels based on the gelation of GO,which is directly initiated using MOF crystals.Free metal ions exposed on the surface of MIL-88A nanorods act as linkers that bind GO nanosheets to a three-dimensional porous network via metal–oxygen covalent or electrostatic interactions.The MOF/rGOderived magnetic and dielectric aerogels Fe_(3)O_(4)@C/rGO and Ni-doped Fe_(3)O_(4)@C/rGO show notable microwave absorption(MA)performance,simultaneously achieving strong absorption and broad bandwidth at low thickness of 2.5(-58.1 dB and 6.48 GHz)and 2.8 mm(-46.2 dB and 7.92 GHz)with ultralow filling contents of 0.7 and 0.6 wt%,respectively.The microwave attenuation ability of the prepared aerogels is further confirmed via a radar cross-sectional simulation,which is attributed to the synergistic effects of their hierarchically porous structures and heterointerface engineering.This work provides an effective pathway for fabricating hierarchically porous MOF/rGO hybrid aerogels and offers magnetic and dielectric aerogels for ultralight MA.