rGO Framework Research Articles

Hybrid Ascharite/Reduced Graphene Oxide with Polysulfide Adsorption Host for Advanced Lithium-Sulfur Batteries.

Balancing the adsorption of lithium-polysulfide intermediates on polar host material surfaces and the effect of their electronic conductivity in the subsequent oxidation and reduction kinetics of electrochemical reactions is necessary and remains a challenge. Herein, we have evaluated the role of polarity and conductivity in preparing a series of ascharite/reduced graphene oxide (RGO) aerogels by dispersing strong polar ascharite nanowires of varying mass into the conductive RGO matrix. When severed as Li-S battery cathodes, the optimized S@ascharite/RGO cathode with a sulfur content of 73.8 wt % demonstrates excellent rate performance and cycle stability accompanied by a high-capacity retention for 500 cycles at 1.0 C. Interesting advantages including the enhanced adsorption ability by the formation of the Mg-S and Li bonds, the continuous and quick electron/ion transportations assembled conductive RGO framework, and the effective deposition of Li2S are combined in the ascharite/RGO aerogel hosts. The electrochemical results further demonstrate that the polarity of ascharite components for the S cathode plays a dominant role in the improvement of electrochemical performance, but the absence of a conductive substrate leads to serious capacity attenuation, especially the rate performance. The balanced design protocol provides a universal method for the synthesis of multiple S hosts for high-performance LSBs.

Foldable chromium vanadate cathodes for high-performance aqueous zinc ion batteries

A novel cathode material, CrV2.7O4.36·2.85H2O/CNT-rGO, composited with a CNT and rGO framework was developed. The flexible battery assembled with it still has stable electrochemical performance under different folding states.

Oriented rGO framework induced hBN confined network in PDMS for absorption enhanced EMI shielding and through-plane thermal conductivity

Herein, inspired by the highly matched phonon spectra between reduced graphene oxide (rGO) and hexagonal boron nitride (hBN), and the good complementarity of the conductive loss of rGO and dielectric loss of hBN in dissipating microwaves, we construct an oriented rGO framework induced hBN confined network in bulk polydimethylsiloxane (PDMS) for electromagnetic interference (EMI) shielding and through-plane thermoconductive properties. A prefabricated three-dimensional (3D) rGO aerogel with a vertically oriented porous structure serving as an electrically conductive framework provides EMI shielding properties, and hBN distributed in the oriented rGO pores constructs a confined through-plane thermoconductive network. The introduction of hBN induces absorption-enhanced EMI shielding through dielectric loss, and the highly matched phonon spectra of rGO and hBN provide more abundant thermal conduction paths and enhance the thermal conductivity of the rGO/hBN/PDMS composites. The synergy of this rGO-hBN dual-network structure gives the composites an excellent EMI shielding effectiveness of 43.1 dB and a good through-plane thermal conductivity of 1.2 W m−1 K−1 at a thickness of 4 mm. This work provides a feasible strategy for realizing shielding and thermoconductive composites with potential applications in next-generation flexible packaging materials.

Quenching-induced construction of graphene-wrapped Fe3O4 composite as ultrahigh-performance Li-storage electrode

Iron oxide/graphene hybrids are outstanding electrodes with high specific capacity for secondary batteries. However, in practice there still remains challenges in alleviating the poor electrical conductivity and significant volume changes of FeOx during the lithiation/delithiation process. Herein, we describe the discovery of fabricating graphene-wrapped Fe3O4 (3D-rGO/Fe3O4) via a solution-based self-assembly process. During which, GO/Fe3O4/Na2SO4 precursor was first formed by the corrosion reaction of metallic Fe in GO aqueous solution and antisolvent self-assembly, which was then quenched into water to dissolve the Na2SO4 template and meanwhile enable the GO to shrink and encapsulate the Fe3O4 nanoparticles spontaneously, followed by a final thermal reduction. Fe3O4 nanoparticles, with a diameter of tens of nanometers, are homogeneously enwrapped into rGO framework, guaranteeing the “plane-to-plane” interconnection. The obtained 3D-rGO/Fe3O4 demonstrates unprecedented Li-storage behaviors when utilized as Li-ion battery anode. Furthermore, quantitative kinetic analysis revealed that both capacitance and diffusion mechanisms account for Li-storage behavior. This contribution not only presents a ultrahigh-performance Li-storage electrode but also shows a novel methodology to design and construct other graghene-based metallic compounds for various applications.

Integrated adsorption and photocatalytic degradation based removal of ciprofloxacin and sulfamethoxazole antibiotics using Fc@rGO-ZnO nanocomposite in aqueous systems

Ferrocene functionalized rGO-ZnO nanocomposite was synthesized via the facile hydrothermal method. ZnO was reduced over the 3-dimensional rGO framework (3D-Fc@rGO) using Camellia sinensis extract. The Fc@rGO-ZnO nanocomposite was employed for pharmaceutical degradation (sulfamethoxazole (SMX) and ciprofloxacin (CIP)) in an aqueous solution under UV C light. The physicochemical properties of the as-prepared photocatalyst were characterized using FTIR, XRD, FESEM, EDS mapping, HR-TEM, XPS, and DR-UV Vis. The as-synthesized Fc@rGO-ZnO photocatalyst performed remarkably against pristine ZnO, with a fivefold increase in removal efficiency. This superior activity was attributed to its improved light harvesting, charge carrier interface, and enhanced charge separation. Additionally, the photocatalyst obeyed the Lagergen model for pseudo-first-order kinetics. Congruously, the integrated approach of Fc@rGO and ZnO as oxidizing agents was proficient in removing >95% of antibiotics (CIP and SMX) within 180 min. Furthermore, the heterostructure configuration developed between Fc@rGO and ZnO helps in charge migration and generation of abundant •OH and •O2− radicals for photodegradation activities. The toxicity assessment of the treated solutions showed improved cell viability in the algal strains of Scenedesmus and Chlorella sp. Moreover, this novel approach for the synthesis of a photoactive nanocomposite is found to be low-cost and reusable for three cycles. The nanocomposite is environmentally sustainable paving the way for practical applications in the treatment of different classes of antibiotics.

Superior electromagnetic wave absorption performances of 3D porous, ultra-thin lightweight BaTiO3@rGO aerogel

Recently, non-magnetic carbon-based composite has been regarded as one of the most promising electromagnetic wave absorbing (EMWA) materials. How to realize high EMWA performances at ultra-thin matching thickness is a hot research topic. In this study, a strategy to construct three-dimensional (3D) porous BaTiO3@reduced graphene oxide (BTO@rGO) composite aerogel was performed by successively hydrothermal process, chemical reduction and freeze-drying. The results show that defect-rich BTO nanoparticles are dispersedly immobilized into 3D conductive rGO framework by a form of Ba2+ bonding to rGO, enhancing conduction loss and dipole polarization, which contributes to enhanced EMWA performance. As a result, a minimum reflection loss of −50.49 dB with a matching thickness of only 1.46 mm, along with an effective absorption bandwidth of 3.74 GHz (13.07 GHz–16.81 GHz) with a matching thickness of only 1.39 mm, is achieved for 3D porous BTO@rGO composite aerogel. Therefore, this study paves a way for designing and preparing excellent non-magnetic EMWA materials at ultra-thin matching thickness.

Bis-terpyridine imprinted nanocage in the confined two-dimensional lamellar membrane for selective adsorption of Nd(III)

Nd is a strategic metal, but its extraction and separation process remains a challenging task. Here, ion-imprinted membranes with six-coordinated and semi-rigid imprinted nanocage structure were developed by self-assembling terpyridine monomers in the confined reduced graphene oxide (rGO) nanochannels. The obtained membranes displayed excellent Nd(III) adsorption capacity of 20.6 mg g−1 in the solution including seven rare earth elements (REEs), together with a 7.68 times higher selectivity to Y(III). Experimental measurements and theoretical calculations revealed that Nd(III) was well coordinated to the six pyridine-nitrogen in the nanocage, which showed shorter average coordination bond (0.77 Å) and stronger binding energy (-10.52 eV) than other REEs. These were mainly attributed to the rigid symmetrical crab-type architecture and specific cavity size of bis-terpyridine nanocage. Meanwhile, the limited decomposition of these metastable nanocage derived from 2D confined effect and nanochannel walls with few groups reduced the interference of groups at non-imprinted sites on selective adsorption. The excellent anti-swelling property of rGO framework endowed 7 static adsorption cycles and maintained high selectivity (K'(Nd/Y) > 7). Integrated into account the well-defined semi-rigid sites constituted by non-covalent interactions, this strategy provided a new idea for facile synthesis of imprinted sites with higher selectivity.

Phase-manipulated hierarchically core-shell Na3(VO1-xPO4)2F1+2x (0≤x≤1)@Na3V2(PO4)3 and its synergistic effect with conformally wrapped reduced graphene oxide framework towards high-performance cathode for sodium-ion batteries

Sodium-ion batteries (SIBs) are regarded as promising candidates for large-scale stationary energy storage systems because of the high abundance of Na resources. Na superionic conductor polyanionic cathode (NASICON), such as Na3(VO1-xPO4)2F1+2x (0 ≤ x ≤ 1, NVPF1+2x) and Na3V2(PO4)3 (NVP), shows intriguing electrochemical performances due to their robust open structure and superior cycle stability. Inspired by phase manipulation and conductive reduced graphene oxide (rGO) incorporation, a hierarchical NVPF1+2x@NVP core-shell structure is elaborately synthesized and conformally wrapped by rGO via a facial microwave-assisted hydrothermal approach. F-free surface of NVPF1+2x@NVP particle possesses intimate contact with rGO framework without strong mutual repulsive force while conductive rGO endows NVPF1+2x@NVP with high electronic conductivity to ensure fast electron transport. Combining the synergistic effect between delicate design of core-shell structure and conductive rGO framework, the NVPF1+2x@NVP/rGO-600 °C electrode achieves a high discharge capacity of 105.9 mAh g−1 at 0.5 C with an impressive capacity retention of 99.1% after 200 cycles, delivering an excellent rate capability of 90.6 mAh g−1 at 10 C. Moreover, the NVPF1+2x@NVP/rGO-600 °C electrode possesses an alleviated polarization, small impedance and fast electron/Na + diffusion properties due to this synergistic effect. The full cell using NVPF1+2x@NVP/rGO-600 °C cathode and hard carbon (HC) anode shows an initial discharge capacity of 80.0 mAh g−1 at 0.2 C and rate capability of 45.2 mAh g−1 at 10 C, which could light an LED lamp and manifest its prospective application. Our findings provide new insights into a broadly applicable material design combining morphological phase manipulation with conductive rGO framework incorporation, which synergistically boosts the electrochemical performance of NASICON cathode towards advanced SIBs with a higher energy density, faster charging rate and more practical applications.

Towering non-Faradaic capacitive storage based on high quality reduced graphene oxide from spent graphite: Direct approach and waste utilization

Urban mining of graphite for higher value addition is considered to be a leading requirement for both the economic and environmental benefits. Herein, we adopted a scalable and novel synthetic approach using modified Hummers method to produce reduced graphene oxide (rGO) directly and graphene oxide (GO) using spent graphite material obtained from scraped Lithium-ion battery (LIB) for the first time. During the synthesis of graphene derivatives, all the metal impurities have been completely terminated through higher temperature oxidation thereby excluding the curing step of graphite. X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FTIR) study clearly manifests that the reduction in lattice d-spacing, absence of impurity phase and removal of oxygen groups confirming the preparation of high-quality rGO framework. The synthesized and thermally reduced GO is used as electrode materials for non-Faradaic super capacitor application in different aqueous electrolytes. In particular, directly synthesized rGO material exhibits the superior capacitance of 156 Fg−1 in neutral system, which is greater than the thermally reduced GO (90 Fg−1) and commercial rGO samples (35 Fg−1). The findings demonstrate that the as-proposed one-pot methodology to produce rGO endows with economic and environmental viability and also exhibits high purity, suitable for several commercial applications at the same time invigorating the worth of graphite conversion from fatigued LIBs.

Facile synthesis of KVPO4F/reduced graphene oxide hybrid as a high-performance cathode material for potassium-ion batteries

Potassium-ion batteries (PIBs) as a substitute for lithium-ion batteries have aroused widespread attention and have been rapidly developed. In the positive electrode materials, polyanionic compound has a high working voltage and large reversible capacity on account of its distinct framework and the strong inducing effect of the anionic group. Herein, a KVPO4F/reduced graphene oxide (KVPF/rGO) hybrid was fabricated via a simple multi-step approach as the polyanionic cathode material for PIBs. Profiting from the small size of KVPF nanoparticles and their uniform distribution in the rGO framework, the as-synthesized KVPF/rGO hybrid manifests a large discharge capacity of 103.2 mAh g−1 with an outstanding energy density of 436.5 Wh kg−1. Through rGO decoration, the hybrid also demonstrates remarkable rate and cycling properties. By employing ex-situ X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) techniques, the potassium storage mechanism of KVPF was clearly revealed. The facile preparation procedure and superior properties endow it great application prospects in large-scale energy storage.

Manipulating the Phase Compositions of Na3(VO1-xPO4)2F1+2x (0 ≤ x ≤ 1) and Their Synergistic Effects with Reduced Graphene Oxide toward High-Rate Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) have aroused intense research and academic interest due to the natural abundance and cost-effectiveness of sodium resources. Presently, cathode materials based on the Na3(VO1-xPO4)2F1+2x (0 ≤ x ≤ 1, NVPF1+2x) polyanionic framework show intriguing electrochemical performances toward practical and advanced SIBs due to its high operating voltage (>3.9 V) and high energy density (>500 Wh kg-1). Different from conventional approaches focusing on delicate morphology design, metal ion substitution, and the conductive matrix's incorporation to overcome the low intrinsic electrical conductivity, here we adopt a one-step microwave-assisted hydrothermal approach to optimize the electrochemical performances of NVPF1+2x via manipulating its phase compositions with different vanadium sources and distinguishing the tetragonal (I4/mmm) symmetry of the Na3(VOPO4)2F phase from the orthorhombic symmetry (Amam) of the Na3V2(PO4)2F3 phase. The introduction of the conductive reduced graphene oxide (rGO) framework and its impacts on the phase compositions were systematically investigated. The rGO framework with different calcination temperature can alter the phase composition and the electrical conductivity of NVPF1+2x cathodes significantly, thus having a great impact on their electrochemical performances. Galvanostatic charge/discharge, cyclic voltammetry, electrochemical impedance spectroscopy, and the galvanostatic intermittent titration technique are adopted to compare their electrode polarization and kinetics difference and show that NVPF@rGO-600 °C possesses a high rate, small polarization, and fast kinetics electrochemical properties. This work provides new insights into manipulating phase compositions of the NVPF1+2x cathode by modulating the synthesis conditions and revealing their synergistic effect with a rGO conductive framework toward a superior rate capability and more realistic practical applications for SIBs.

Synthesis of Si/Fe2O3-Anchored rGO Frameworks as High-Performance Anodes for Li-Ion Batteries.

By virtue of the high theoretical capacity of Si, Si-related materials have been developed as promising anode candidates for high-energy-density batteries. During repeated charge/discharge cycling, however, severe volumetric variation induces the pulverization and peeling of active components, causing rapid capacity decay and even development stagnation in high-capacity batteries. In this study, the Si/Fe2O3-anchored rGO framework was prepared by introducing ball milling into a melt spinning and dealloying process. As the Li-ion battery (LIB) anode, it presents a high reversible capacity of 1744.5 mAh g−1 at 200 mA g−1 after 200 cycles and 889.4 mAh g−1 at 5 A g−1 after 500 cycles. The outstanding electrochemical performance is due to the three-dimensional cross-linked porous framework with a high specific surface area, which is helpful to the transmission of ions and electrons. Moreover, with the cooperation of rGO, the volume expansion of Si is effectively alleviated, thus improving cycling stability. The work provides insights for the design and preparation of Si-based materials for high-performance LIB applications.

Self-assembly of antimony sulfide nanowires on three-dimensional reduced GO with superior electrochemical lithium storage performances

The three-dimensional Sb2S3 nanowires/reduced graphene oxide (SBSWs/rGO) was prepared as an anode for lithium storage by self-assembling SBSWs on 3D rGO framework. SBSWs/rGO shows the perfect rate capability (505 mAh g−1 at 3 A g−1) and long cycle stability (697 mAh g−1 after 100 cycles at 100 mA g−1). The 3D rGO framework has good structural stability, which can provide a free space towards shortening lithium ions diffusion paths and accommodating the volume change of SBSWs. The rGO sheets with high electrical conductivity promote electron transfer in composites to improve rate performances.

Design of best performing hexagonal shaped Ag@CoS/rGO nanocomposite electrode material for electrochemical supercapacitor application

Abstract The mixed metal/metal sulphide (Ag@CoS) with reduced graphene oxide (rGO) nanocomposite (Ag@CoS/rGO) was synthesized for the possible electrode in supercapacitors. Ag@CoS was successfully deposited on the rGO nanosheets by hydrothermal method, implying the growth of 2D Ag and CoS-based hexagonal-like structure on the rGO framework. The synthesized nanocomposite was subjected to structural, morphological and electrochemical studies. The XRD results show that the prepared nanocomposite material exhibits a combination of hexagonal and cubic phase due to the presence of CoS and Ag phases together. The band appearing at nearly 470.33 cm−1 in FTIR spectra can be ascribed to the absorption of S–S bond in the Ag@CoS/rGO nanocomposite. The clear hexagonal structure was analysed by SEM and TEM with the grain sizes ranging from nanometer to micrometer. The electrode material exhibits excellent cyclic stability with a specific capacitance of 1580 F/g at a current density of 0.5 A/g without any loss of capacitive retention even after 1000 cycles. Based on the electrochemical performance, it can be inferred that the prepared novel nanocomposite material is very suitable for using as an electrode for electrochemical supercapacitor applications.

Synthesis of a pomegranate shaped reduced graphene oxide stabilized secondary Si nanoparticles composite anode for lithium ion batteries

A 3D porous micro-size pomegranate shaped nano-silicon and reduced graphene oxide composite (Si/RGO-S) is synthesized in this work by spray drying and magnesiothermic reduction treatments of silicon dioxides (SiO2) nanospheres and few-layered graphene oxide sheets (GO). The SiO2 nanospheres convert to smaller Si secondary nanocrystals and GO sheets are deoxygenated to form a supporting RGO framework, respectively. Favorable void space is created between the secondary Si nanoparticles for the accommodation of the volume changes during lithium ion storage. The 3D porous RGO protecting skeleton not only improves the overall electronic and ionic conductivity, but also effectively immobilizes the inside Si nanoparticles. Under a current density of 500 mA g−1, the 3D Si/RGO-S composite exhibits a reversible capacity of 1200 mAh g−1 for 300 consecutive cycles, which is much higher than the controlled 2D sample (Si/RGO-F) prepared by a freeze drying and magnesiothermic reduction method as anode material for lithium ion batteries. The insight into the superior lithium ion storage performance of the Si/RGO-S has been given in this work.

Photocatalytic TiO2/rGO/CuO Composite for Wastewater Treatment of Cr(VI) Under Visible Light

The harm of chromium pollution to the environment has caused a widespread concern; hexavalent chromium is a toxic, cancerogenic, and genetically mutagenic contaminant to the human body; by contrast, trivalent chromium is almost non-toxic to the human body; therefore, it is a feasible method to reduce hexavalent chromium to trivalent chromium. Photocatalysis is a new environmentally friendly and harmless technology, which can transform pollutants into non-toxic or less toxic products. In this study, we synthesized TiO2/rGO/CuO ternary nanocomposites to treat hexavalent chromium pollution under visible light. Under optimal conditions, the photoreduction efficiency of 100 ppm hexavalent chromium solution could reach 100% in 80 min. The photoreduction rate of hexavalent chromium is 29.4 times than that of pure TiO2. The photocatalytic property of CuO in TG2C8 nanocomposites is attributed to accelerate the separation of electrons and holes and the efficient electron transfer through the rGO framework. We believe that TiO2/rGO/CuO composites have great potential in wastewater treatment.

Implication of Three Dimensional Framework Architecture of Graphitic Carbon Nanosheets for Improving Electrical Conductivity Under Mechanical Deformation

In this study, based on three-dimensional (3D) framework architecture built-up with two-dimensional (2D) graphitic carbon such as graphene, we have prepared a mechanically robust polymer composite without exhibiting notable deterioration of electrical conductivity under mechanical deformation. In constructing 3D framework comprising of graphitic carbons, two sophisticated methodologies, direct formation of graphitic layers on metal foam by chemical vapor deposition (CVD), and lay-up of reduced graphene oxide (rGO) nanosheets on metal foam have been performed, respectively, and their sustainability of conductive performance under mechanical deformation has been comparatively examined in terms of electrical conductivity change by cyclic mechanical stress. The CVD-synthesized graphene (CGr) framework-embedded PDMS composite, which means a PDMS composite containing 3D graphene framework grown by CVD process, exhibited electrical conductivity of ∼5 S/m at graphene content of 1.0 wt%, which was ∼5 orders of magnitude higher than that of 3D rGO framework-embedded PDMS composite containing comparable loading of rGO. When subjected to repetitive mechanical stress, it was found that the superior conductivity performance of CGr framework over rGO framework was well retained, presumably due to the higher perfectness of graphitic layers, which would impart much longer electron transfer to the framework architecture of graphitic carbon nanosheets.

Nanostructuring of pseudocapacitive MnFe2O4/Porous rGO electrodes in capacitive deionization

Capacitive deionization (CDI) has been used to remove salt ions with carbon electrodes by the electrical double layer (EDL) mechanism. Other non-carbon materials based on pseudocapacitive mechanism resulting from faradaic reactions with fast electrosorption/desorption properties have emerged as new promising electrode materials. Until now, pseudocapacitive behavior was limited to thin film electrodes with nanometer thickness and was not yet suitable for practical application. In this work, we employed a two-times of hydrothermal synthesis process constructing MnFe2O4/Porous rGO (MFO/PrGO) nanostructure as pseudocapacitive electrodes. In this carefully designed architecture, the dense structure of MFO/rGO prepared by first-time hydrothermal process provided good connections of MFO nanoparticle with rGO framework for efficient redox charge transfer; the chemically-etched porous rGO used in the second-time hydrothermal process offered hierarchical pores for easier access of the electrode materials, both contributed in enhanced pseudocapacitive electrosorption. HRTEM verified the MnFe2O4 spinel structure and measured the inter-planar lattice parameter which functioned for ion intercalating in and out of the electrode. The MFO/PrGO electrode resulted in 237 F/g in electrosorption of ions from aqueous solution which was higher than the MFO only electrode. Finally, in the CDI experiment, the great salt electrosorption capacity of 8.9 mg/g and 100% regeneration in multiple cycles were achieved by the MFO/PrGO nanocomposite electrode. These results paved the way for using spinel compounds and graphene nanocomposite electrodes for efficient electrosorption and desalination.

Self-supporting porous CoS2/rGO sulfur host prepared by bottom-up assembly for lithium-sulfur batteries

Cobalt disulfide (CoS2) has been revealed as strong adsorption and activation sites for polar polysulfides, which effectively accelerates the redox reactions of polysulfides in lithium-sulfur (Li-S) batteries. As an ideal sulfur host, a three-dimensional (3D) graphene framework is adopted for high-performance Li-S batteries. Considering the special function of the CoS2 nanoparticles and the advantages of a 3D porous graphene framework, a porous CoS2/reduced graphene oxide (CoS2/rGO) binder-free sulfur host is prepared by a bottom-up assembly and hydrothermal treatment. The porous rGO film is stacked by interconnected graphene sheets, and the CoS2 nanoparticles are dispersed on the graphene sheets uniformly, which effectively obstructs the stacking of graphene sheets. As a binder-free sulfur host, the porous CoS2/rGO sulfur host combines the sufficient electron conductivity of the porous rGO framework and the sulfur immobilization interaction of the CoS2 nanoparticles. This host material demonstrates an initial discharge capacity of 993.5 mAh g−1 and a capacity of 806.7 mAh g−1 after 110 cycles at 0.5 C. Both the capacity and cycling stability of the CoS2/rGO cathode were greatly improved over that of rGO. Furthermore, the bottom-up assembly approach provides a novel opportunity for preparing self-supporting graphene-based nanocomposite electrodes.

FeCo-Anchored Reduced Graphene Oxide Framework-Based Soft Composites Containing Carbon Nanotubes as Highly Efficient Microwave Absorbers with Excellent Heat Dissipation Ability.

Conducting polymer composites containing ferromagnetic grafted-graphene derivatives are already appreciated for their lightweight, flexibility, and cost effectiveness in terms of microwave absorption. To further leverage the said properties of this wonder material, we propose a highly efficient replacement by blending conducting multiwall carbon nanotube (MWCNT) and FeCo anchored covalent cross-linked reduced graphene oxide (rGO) with poly(vinylidene fluoride) (PVDF). Interconnected conducting network of MWCNTs introduces higher electrical conductivity in the blend which is essential for microwave absorption. FeCo-anchored porous interconnected rGO framework was designed via solvent-mediated in situ coreduction in the presence of Fe(II) and Co(II) precursors. Resulting cross-linked-rGO/FeCo displays fascinating coexistence of ferromagnetism and conducting-dielectric behavior, while largely preserving the robust 3D porous interconnected structure. Coupled with conducting MWCNTs, diamine cross-linked rGO/FeCo in a soft polymer matrix yields remarkably high total shielding effectiveness (SET) of -41.2 dB at 12 GHz, for a meager 10 wt % filler content. In addition, the composite materials display efficient heat dissipation abilities in conjunction with the trend in their thermal conductivities. This new-age microwave-absorbing material, powered by multifunctionality and tunable magnetodielectric properties, henceforth offers an amendable, cost-effective replacement to the existing solutions.