Metal–Organic Gel Leading to Customized Magnetic‑Coupling Engineering in Carbon Aerogels for Excellent Radar Stealth and Thermal Insulation Performances

Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic hydrogels are prepared by regulating the complexation effect,solution polarity and curing speed.Meanwhile,collagen peptide is used to facilitate the fabrication of a porous aerogel with excellent physical properties as well as the homogeneous dispersion of magnetic particles during calcination.Subsequently,two kinds of heterometallic magnetic coupling systems are obtained through the application of Kirkendall effect.FeCo/nitrogen-doped carbon(NC)aerogel demonstrates an ultra-strong microwave absorption of−85 dB at an ultra-low loading of 5%.After reducing the time taken by atom shifting,a FeCo/Fe3O4/NC aerogel containing virus-shaped particles is obtained,which achieves an ultra-broad absorption of 7.44 GHz at an ultra-thin thickness of 1.59 mm due to the coupling effect offered by dual-soft-magnetic particles.Furthermore,both aerogels show excellent thermal insulation property,and their outstanding radar stealth performances in J-20 aircraft are confirmed by computer simulation technology.The formation mechanism of MOG is also discussed along with the thermal insulation and electromagnetic wave absorption mechanism of the aerogels,which will enable the development and application of novel and lightweight stealth coatings.

From VIB‑to VB‑Group Transition Metal Disulfides:Structure Engineering Modulation for Superior Electromagnetic Wave Absorption

The laminated transition metal disulfides(TMDs),which are well known as typical two-dimensional(2D)semiconductive materials,possess a unique layered structure,leading to their wide-spread applications in various fields,such as catalysis,energy storage,sensing,etc.In recent years,a lot of research work on TMDs based functional materials in the fields of electromagnetic wave absorption(EMA)has been carried out.Therefore,it is of great significance to elaborate the influence of TMDs on EMA in time to speed up the application.In this review,recent advances in the development of electromagnetic wave(EMW)absorbers based on TMDs,ranging from the VIB group to the VB group are summarized.Their compositions,microstructures,electronic properties,and synthesis methods are presented in detail.Particularly,the modulation of structure engineering from the aspects of heterostructures,defects,morphologies and phases are systematically summarized,focusing on optimizing impedance matching and increasing dielectric and magnetic losses in the EMA materials with tunable EMW absorption performance.Milestones as well as the challenges are also identified to guide the design of new TMDs based dielectric EMA materials with high performance.

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.

Self-Healing Liquid Metal Magnetic Hydrogels for Smart Feedback Sensors and High-Performance Electromagnetic Shielding

Hydrogels exhibit potential applications in smart wearable devices because of their exceptional sensitivity to various external stimuli.However,their applications are limited by challenges in terms of issues in biocompatibility,custom shape,and self-healing.Herein,a conductive,stretchable,adaptable,self-healing,and biocompatible liquid metal GaInSn/Ni-based composite hydrogel is developed by incorporating a magnetic liquid metal into the hydrogel framework through crosslinking polyvinyl alcohol(PVA)with sodium tetraborate.The excellent stretchability and fast self-healing capability of the PVA/liquid metal hydrogel are derived from its abundant hydrogen binding sites and liquid metal fusion.Significantly,owing to the magnetic constituent,the PVA/liquid metal hydrogel can be guided remotely using an external magnetic field to a specific position to repair the broken wires with no need for manual operation.The composite hydrogel also exhibits sensitive deformation responses and can be used as a strain sensor to monitor various body motions.Additionally,the multifunctional hydrogel displays absorption-dominated electromagnetic interference(EMI)shielding properties.The total shielding performance of the composite hydrogel increases to~62.5 dB from~31.8 dB of the pure PVA hydrogel at the thickness of 3.0 mm.The proposed bioinspired multifunctional magnetic hydrogel demonstrates substantial application potential in the field of intelligent wearable devices.

Hierarchical Magnetic Network Constructed by CoFe Nanoparticles Suspended Within “Tubes on Rods” Matrix Toward Enhanced Microwave Absorption

Hierarchical magnetic-dielectric composites are promising functional materials with prospective applications in microwave absorption(MA)field.Herein,a three-dimension hierarchical“nanotubes on microrods,”core–shell magnetic metal–carbon composite is rationally constructed for the first time via a fast metal–organic frameworksbased ligand exchange strategy followed by a carbonization treatment with melamine.Abundant magnetic CoFe nanoparticles are embedded within one-dimensional graphitized carbon/carbon nanotubes supported on micro-scale Mo2N rod(Mo2N@CoFe@C/CNT),constructing a special multi-dimension hierarchical MA material.Ligand exchange reaction is found to determine the formation of hierarchical magnetic-dielectric composite,which is assembled by dielectric Mo2N as core and spatially dispersed CoFe nanoparticles within C/CNTs as shell.Mo2N@CoFe@C/CNT composites exhibit superior MA performance with maximum reflection loss of−53.5 dB at 2 mm thickness and show a broad effective absorption bandwidth of 5.0 GHz.The Mo2N@CoFe@C/CNT composites hold the following advantages:(1)hierarchical core–shell structure offers plentiful of heterojunction interfaces and triggers interfacial polarization,(2)unique electronic migration/hop paths in the graphitized C/CNTs and Mo2N rod facilitate conductive loss,(3)highly dispersed magnetic CoFe nanoparticles within“tubes on rods”matrix build multi-scale magnetic coupling network and reinforce magnetic response capability,confirmed by the off-axis electron holography.

MOF-Derived Ni1-xCox@Carbon with Tunable Nano-Microstructure as Lightweight and Highly Efficient Electromagnetic Wave Absorber

Intrinsic electric-magnetic property and special nano-micro architecture of functional materials have a significant effect on its electromagnetic wave energy conversion,especially in the microwave absorption(MA) field.Herein,porous Ni1-xCox@Carbon composites derived from metal-organic framework(MOF)were successfully synthesized via solvothermal reaction and subsequent annealing treatments.Benefiting from the coordination,carbonized bimetallic Ni-Co-MOF maintained its initial skeleton and transformed into magnetic-carbon composites with tunable nano-micro structure.During the thermal decomposition,generated magnetic particles/clusters acted as a catalyst to promote the carbon sp^2 arrangement,forming special core-shell architecture.Therefore,pure Ni@C microspheres displayed strong MA behaviors than other Ni1-xCox@Carbon composites.Surprisingly,magnetic-dielectric Ni@C composites possessed the strongest reflection loss value-59.5 dB and the effective absorption frequency covered as wide as 4.7 GHz.Meanwhile,the MA capacity also can be boosted by adjusting the absorber content from 25% to 40%.Magnetic-dielectric synergy effect of MOF-derived Ni1-xCox@Carbon microspheres was confirmed by the off-axis electron holography technology making a thorough inquiry in the MA mechanism.

Recent Advances in Design Strategies and Multifunctionality of Flexible Electromagnetic Interference Shielding Materials

With rapid development of 5G communication technologies,electromagnetic interference(EMI)shielding for electronic devices has become an urgent demand in recent years,where the development of corresponding EMI shielding materials against detrimental electromagnetic radiation plays an essential role.Meanwhile,the EMI shielding materials with high flexibility and functional integrity are highly demanded for emerging shielding applications.Hitherto,a variety of flexible EMI shielding materials with lightweight and multifunctionalities have been developed.In this review,we not only introduce the recent development of flexible EMI shielding materials,but also elaborate the EMI shielding mechanisms and the index for"green EMI shielding"performance.In addition,the construction strategies for sophisticated multifunctionalities of flexible shielding materials are summarized.Finally,we propose several possible research directions for flexible EMI shielding materials in near future,which could be inspirational to the fast-growing next-generation flexible electronic devices with reliable and multipurpose protections as offered by EMI shielding materials.

3D Seed-Germination-Like MXene with In Situ Growing CNTs/Ni Heterojunction for Enhanced Microwave Absorption via Polarization and Magnetization

Ti_(3)C_(2)Tx MXene is widely regarded as a potential micro-wave absorber due to its dielectric multi-layered structure.However,missing magnetic loss capability of pure MXene leads to the unmatched electromagnetic parameters and unsatisfied impedance matching condi-tion.Herein,with the inspiration from dielectric-magnetic synergy,this obstruction is solved by fabricating magnetic CNTs/Ni hetero-structure decorated MXene substrate via a facile in situ induced growth method.Ni2+ions are successfully attached on the surface and interlamination of each MXene unit by intensive electrostatic adsorption.Benefiting from the possible“seed-germination”effect,the“seeds”Ni^(2+)grow into“buds”Ni nanoparticles and“stem”carbon nanotubes(CNTs)from the enlarged“soil”of MXene skeleton.Due to the improved impedance matching con-dition,the MXene-CNTs/Ni hybrid holds a superior microwave absorp-tion performance of−56.4 dB at only 2.4 mm thickness.Such a distinctive 3D architecture endows the hybrids:(i)a large-scale 3D magnetic coupling network in each dielectric unit that leading to the enhanced magnetic loss capability,(ii)a massive multi-heterojunction interface structure that resulting in the reinforced polarization loss capability,confirmed by the off-axis electron holography.These outstanding results provide novel ideas for developing magnetic MXene-based absorbers.

One-Dimensional Magnetic FeCoNi Alloy Toward Low-Frequency Electromagnetic Wave Absorption

Rational designing of one-dimensional(1D)magnetic alloy to facilitate electromagnetic(EM)wave attenuation capability in low-frequency(2-6 GHz)microwave absorption field is highly desired but remains a significant challenge.In this study,a composite EM wave absorber made of a FeCoNi medium-entropy alloy embedded in a 1D carbon matrix framework is rationally designed through an improved electrospinning method.The 1D-shaped FeCoNi alloy embedded composite demonstrates the high-density and continuous magnetic network using off-axis electronic holography technique,indicating the excellent magnetic loss ability under an external EM field.Then,the in-depth analysis shows that many factors,including 1D anisotropy and intrinsic physical features of the magnetic medium-entropy alloy,primarily contribute to the enhanced EM wave absorption performance.Therefore,the fabricated EM wave absorber shows an increasing effective absorption band of 1.3 GHz in the low-frequency electromagnetic field at an ultrathin thickness of 2 mm.Thus,this study opens up a new method for the design and preparation of high-performance 1D magnetic EM absorbers.

Self‑Assembly MXene‑rGO/CoNi Film with Massive Continuous Heterointerfaces and Enhanced Magnetic Coupling for Superior Microwave Absorber

MXene, as a rising star of two-dimensional(2 D) materials, has been widely applied in fields of microwave absorption and electromagnetic shielding to cope with the arrival of the 5 G era. However, challenges arise due to the excessively high permittivity and the difficulty of surface modification of few-layered MXenes severely, which infect the microwave absorption performance. Herein, for the first time, a carefully designed and optimized electrostatic selfassembly strategy to fabricate magnetized MXene-r GO/Co Ni film was reported. Inside the synthesized composite film, r GO nanosheets decorated with highly dispersed Co Ni nanoparticles are interclacted into MXene layers, which effectively suppresses the originally self-restacked of MXene nanosheets, resulting in a reduction of high permittivity. In addition, owing to the strong magnetic coupling between the magnetic Fe Co alloy nanoparticles on the r GO substrate, the entire MXener GO/Co Ni film exhibits a strong magnetic loss capability. Moreover, the local dielectric polarized fields exist at the continuous heterointerfaces between 2 D MXene and r GO further improve the capacity of microwave loss. Hence, the synthesized composite film exhibits excellent microwave absorption property with a maximum reflection loss value of-54.1 d B at 13.28 GHz. The electromagnetic synergy strategy is expected to guide future exploration of high-efficiency MXene-based microwave absorption materials.

Ultrahigh Density of Atomic CoFe-Electron Synergy in Noncontinuous Carbon Matrix for Highly Efficient Magnetic Wave Adsorption

Improving the atom utilization of metals and clarifying the M–M’interaction is both greatly significant in assembling high-performance ultra-light electromagnetic wave-absorbing materials.Herein,a high-temperature explosion strategy has been successfully applied to assemble the hierarchical porous carbon sponge with Co–Fe decoration via the pyrolysis of the energetic metal organic framework.The as-constructed hybrid displays a superior reflection loss(RL)value of-57.7 d B and a specific RL value of-192 d B mg-1 mm-1 at 12.08 GHz with a layer thickness of 2.0 mm(loading of 15 wt%).The off-axis electron hologram characterizes the highly distributed numerous polarized nanodomain variable capacitors,demonstrating the dipole and interfacial polarization along the edges of the nanopores.More importantly,the X-ray absorption spectroscopy analysis verifies the mutual interaction between the metal cluster and carbon matrix and the electronic coupling responsible for the greatly improved electromagnetic wave absorption.

Measurement of the remnant magnetic-field in Lorentz mode using permalloy

A novel method was reported to measure the remnant magnetic field in Lorentz mode in a FEI Tecnai F20 transmission electron microscope equipped with a Lorentz lens. The movement of the circle Bloch line of the cross-tie wall in Permalloy is used to measure the remnant magnetic field by tilting the specimen and adjusting the objective lens current. The remnant magnetic field is estimated to be about 17 Oe, in a direction opposite to that of the objective lens magnetic field. The remnant magnetic field can be compensated by adjusting the value of the objective lens current.

Phase transition of magnetic skyrmion by Lorentz transmission electron microscopy

Magnetic skyrmion has launched new concepts for memory devices due to its topologically vortex-like magnetic structure.Here,we report the first experimental observation of the skyrmion chain in Fe Ge nanostripes by using high resolution Lorentz transmission electron microscopy.Under an applied field,we observe that the helical ground states

Hollow FeCoNiAl microspheres with stabilized magnetic properties for microwave absorption

Development of high-performance microwave absorption materials(MAM)with stabilized magnetic properties at high temperatures is specifically essential but remains challenging.Moreover,the Snoke's limitation restrains the microwave absorption(MA)property of magnetic materials.Modulating alloy components is considered an effective way to solve the aforementioned problems.Herein,a hollow medium-entropy FeCoNiAl alloy with a stable magnetic property is prepared via simple spray-drying and two-step annealing for efficient MA.FeCoNiAl exhibited an ultrabroad effective absorption band(EAB)of 5.84 GHz(12.16–18 GHz)at a thickness of just 1.6 mm,revealing an excellent absorption capability.Furthermore,the MA mechanism of FeCoNiAl is comprehensively investigated via off-axis holography.Finally,the electromagnetic properties,antioxidant properties,and residual magnetism at high temperatures of FeCoNiAl alloys are summarized in detail,providing new insights into the preparation of MAM operating at elevated temperatures.

Engineering the electronic structure on MXenes via multidimensional component interlayer insertion for enhanced electromagnetic shielding

MXene-based functional electromagnetic interference(EMI)shielding films are highly desirable for mod-ern integrated electronic and telecommunication systems in aerospace,military,artificial intelligence,and smart and wearable electronics field.In this work,3D freestanding Ti_(3)C_(2)T_(x)/CNTs/Ni film assembled by 1D multi-walled carbon nanotubes(MWCNTs)/Ni and 2D Ti_(3)C_(2)T_(x)MXene sheets was synthesized by a facile vacuum filtration process.By electrostatic incorporation,hexagonal nickel plates embed on the CNTs and then the CNTs/Ni insert into the Ti_(3)C_(2)T_(x)layers to form magnetized Ti_(3)C_(2)T_(x)-based functional film with a compact and laminated structure.Due to the outstanding electron migration capacity in the highly conductive Ti_(3)C_(2)T_(x)sheet and multiple internal reflections from porous and segregated structures,the op-timized Ti_(3)C_(2)T_(x)/CNTs/Ni composite films show excellent EMI shielding effectiveness of 67.4 dB with elec-trical conductivity of 744 S cm^(-1).Surprisingly,a magnetization compensation strategy is built to boost the EMI shielding effectiveness with decreased conductivity.Meanwhile,the visual magnetic coupling phenomenon and charge distribution in the heterogeneous interfaces could be observed in the recon-structed electron holography images.Those encouraging results shed light on novel magnetized MXene-based functional films for high-performance EMI shielding.

Direct imaging of stress-induced magnetic behavior transitions

Stress induction plays a special role in performance control for material science.So far,it has remained challenging to systematically investigate magnetoelectric effect under stress-mediated interaction.Here we constructed a magnetoelectric device with piezoelectric stress induction,in which the stress plays a crucial intermediate role during the controllable modification of the magnetic behavior transitions under the magnetic field or current pulse driven process.The compressive stress was found to make the above process easier and reduce energy consumption via changing the magnetic domain energy state.Meanwhile,both the domain distribution and domain-wall driven process are sensitive to stress intensity.Our magnetoelectric device integrated the advantages of voltage-stress and spin-current for the control of magnetic behavior transition with the help of micro-nano processing.For the stress-induced magnetic behavior in magnetic materials was directly imaged and quantificationally investigated,the complex interactions between stress,magnetic domain motion,magnetic field,and spin current have been clarified.

A direct H2O2 production based on hollow porous carbon sphere-sulfur nanocrystal composites by confinement effect as oxygen reduction electrocatalysts

Carbon-sulfur composites have draw n in creasing interest in various fields including electrocatalysis because of their unique structures.However,carb on-sulfur composite with tiny sulfur nano crystals has still received little attention.Herein,hollow porous carb on sphere-sulfur composite(HPCS-S)which possesses excellent electrochemical performance towards H2O2 has been prepared for the first time via a simple silica template method.The 2-5 nm sulfur nan ocrystals being restricted in the cha nnel of the hollow porous carb on spheres are un der a strong compressive stress,which was further con firmed by high-resoluti on tran smissi on electr on microscopy(HRTEM)and GPA.The HPCS-S nano crystals show better con ductivity tha n amorphous sulfur clusters because of the reducti on of the steric hindrance which efficie ntly promotes the electron transportation.Consequently,the higher activity and selectivity towards the 2e^oxygen reduction reaction(ORR)to H2O2 in alkaline solution was obtained.The H2O2 selectivity rises from 20%to over 70%after the sulfur addition and the H2O2 production rate achieves 183.99 mmol-gcataiyst-1 with the Faradaic efficiency of 70%.Furthermore,performance enhancement mechanism was also investigated using the den sity functional theory(DFT)calculatio ns.After the in troduci ng of sulfur nano crystals,the appeara nee of S-S bond greatly decreases the overpotential compared with S-doping,which results in significant enhancement of the electrocatalytic property.Consequently,the HPCS-S can be an efficient H2O2 production electrocatalyst in alkaline solution.

Growth of magnetic metals on carbon microspheres with synergetic dissipation abilities to broaden microwave absorption

Microwave absorption(MA) materials have been captured extensive attentions due to the serious electromagnetic(EM) pollution. Numerous interests focus on the MA performances of core-shell structural composites with magnetic constituents as cores and dielectric constituents as shells, which inevitably suppressed the magnetic coupling causing the decrease of magnetic loss to some extent. Herein, the coreshell structural carbon(C) microsphere/magnetic metal composites were fabricated through the combination of an electrostatic assembly approach and subsequent in-situ reduction reaction. The complex permittivity and permeability of core-shell C@magnetic metal composite system can be effective adjusted by the constituent and microstructure of shells. Thanks to the distinct magnetic coupling from the subtle designed structures and the promotion of the magnetic-dielectric synergy, the C@magnetic metal composite exhibited enhanced MA properties. The optimal reflection loss(RL) of C@Ni composite was-54.1 dB with a thickness of 3.4 mm, meanwhile the effective absorbing band could reach over 5.5 GHz at only a1.8 mm thickness. Broad absorption bandwidth with RL below-10 d B could achieve 6.0 GHz and 6.7 GHz for C@Co and C@Ni Co composites with a thin 2.1 mm thickness, respectively. Our exciting findings might lead a guide on the novel structure design for the functional core-shell structural composites used for microwave absorption.

Self-transforming ultrathin α-Co(OH)2 nanosheet arrays from metal-organic framework modified graphene oxide with sandwichlike structure for efficient electrocatalytic oxygen evolution

Developing efficient and low-cost electrocatalysts for oxygen evolution reaction(OER)with high electrochemical activity and durability for diverse renewable and sustainable energy technologies remains challenging.Herein,an ultrasonic-assisted and coordination modulation strategy is developed to construct sandwich-like metal-organic framework(MOF)derived hydroxide nanosheet(NS)arrays/graphene oxide(GO)composite via one-step self-transformation route.Inducing from unsteady state,the dodecahedral ZIF-67 with Co^2+in tetrahedral coordination auto-converts into defect-rich ultrathin layered hydroxides with the interlayered ion NO3-.The self-transforming a-Co(OH)2/GO nanosheet arrays from ZIF-67(Co(OH)2-GNS)change the coordination mode of Co^2+and bring about the exposure of more metal active sites,thereby enhancing the spatial utilization ratio within the framework.As monometal-based electrocatalyst,the optimized Co(OH)2-GNS exhibits remarkable OER catalytic performance evidenced by a low overpotential of 259 mV to achieve a current density of 10 mA·cm-2 in alkaline medium,even exceeding commercial RuO2.During the oxygen evolution process,electron migration can be accelerated by the interfacial/in-plane charge polarization and local electric field,corroborated by the off-axis electron holography.Density functional theory(DFT)calculations further studied the collaboration between ultrathin Co(OH)2 NS and GO,which leads to lower energy barriers of intermediate products and greatly promotes electrocatalytic property.

Boosting oxygen reduction activity of spinel CoFe2O4 by strong interaction with hierarchical nitrogen-doped carbon nanocages

The unique hierarchical nitrogen-doped carbon nanocages(h NCNC) are used as a new support to homogeneously immobilize spinel Co Fe_2O_4 nanoparticles by a facile solvothermal method. The so-constructed hierarchical Co Fe_2O_4/h NCNC catalyst exhibits a high oxygen reduction activity with an onset potential of0.966 V and half-wave potential of 0.819 V versus reversible hydrogen electrode, far superior to the corresponding 0.846 and 0.742 V for its counterpart of Co Fe_2O_4/h CNC with undoped hierarchical carbon nanocages(h CNC) as the support, which locates at the top level for spinel-based catalysts to date.Consequently, the Co Fe_2O_4/h NCNC displays the superior performance to the Co Fe_2O_4/h CNC, when used as the cathode catalysts in the home-made Al-air batteries. X-ray photoelectron spectroscopy characterizations reveal the more charge transfer from Co Fe_2O_4 to h NCNC than to h CNC, indicating the stronger interaction between Co Fe_2O_4 and h NCNC due to the nitrogen participation. The enhanced interaction and hierarchical morphology favor the high dispersion and modification of electronic states for the active species as well as the mass transport during the oxygen reduction process, which plays a significant role in boosting the electrocatalytic performances. In addition, we noticed the high sensitivity of O 1 s spectrum to the particle size and chemical environment for spinel oxides, which is used as an indicator to understand the evolution of ORR activities for all the Co Fe_2O_4-related contrast catalysts. Accordingly,the well-defined structure-performance relationship is demonstrated by the combination of experimental characterizations with theoretical calculations. This study provides a promising strategy to develop efficient, inexpensive and durable oxygen reduction electrocatalysts by tuning the interaction between spinel metal oxides and the carbon-based supports.