Regulating the coordination microenvironment of atomic bismuth sites in nitrogen-rich carbon nanosheets as anode for superior potassium-ion batteries

Carbon-based materials are recognized as anodes fulling of promise for potassium ion batteries(PIBs)due to advantages of affordable cost and high conductivity.However,they still face challenges including structural unstability and slow kinetics.It is difficult to achieve efficient potassium storage with unmodified carbonaceous anode.Herein,atomic bismuth(Bi)sites with different atom coordinations anchored on carbon nanosheets(CNSs)have been synthesized through a template method.The properties of prepared multi-doping carbon anodes Bi-N_(3)S_(1)/CNSs,Bi-N_(3)P_(1)/CNSs and Bi-N_(4)/CNSs were probed in PIBs.The configuration Bi-N_(3)S_(1) with stronger charge asymmetry exhibits superior potassium storage performance compared to Bi-N_(3)P_(1) and Bi-N_(4) configurations.The Bi-N_(3)S_(1)/CNSs display a rate capacity of 129.2 mAh g^(-1)even at 10 A g^(-1)and an impressive cyclability characterized by over 5000 cycles at 5 A g^(-1),on account of its optimal coordination environment with more active Bi centers and K^(+)adsorption sites.Notably,assembled potassium-ion full cell Mg-KVO//Bi-N_(3)S_(1)/CNSs also shows an outstanding cycling stability,enduring 3000 cycles at 2 A g^(-1).Therefore,it can be demonstrated that regulating the electronic structure of metallic centre M-N_(4) via changing the type of ligating atom is a feasible strategy for modifying carbon anodes,on the base of co-doping metal and non-metal.

Reusable salt-template strategy for synthesis of porous nitrogen-rich carbon boosts H_(2)S selective oxidation

Removing hydrogen sulfide(H_(2)S)via the selective oxidation has been considered an effective way to further purify the indusial sulfurcontaining due to it can completely transform residual H_(2)S into elemental sulfur.While N-doped porous carbon was applied to H_(2)S selective oxidation,a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty,limiting its future development in large-scale applications.Herein,we present porous,honeycomb-like N-doped carbon catalysts with large specific surface areas,high pyridinic N content,and numerous structural defects for H_(2)S selective oxidation prepared using reusable NaCl as the template.The asprepared NC-10-800 catalyst exhibits excellent catalytic performance(sulfur formation rate of 784 g_(sulfur) kg_(cat.)^(-1) h^(-1)),outstanding stability(>100 h),and excellent anti-water vapor,anti-CO_(2) and anti-oxidation properties,suggesting significant potential for practical industrial application.The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity.Importantly,the water-soluble NaCl template could be easily washed from the carbon nanomaterials,and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors.This environment-friendly,low-cost,reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.

Nitrogen-rich carbon for catalytic activation of peroxymonosulfate towards green synthesis

Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-C due to the thermodynamic instability of C-N skeleton.In this study,we proposed an innovative epitaxial growth approach to synthesize two-dimensional N-C nanosheets.Leveraging the abundant amino groups supplied by the polymer dots as growing sites,we successfully attained a high nitrogen level and spontaneously introduced abundant structural defects in the carbon framework.The resulting N-C nanosheets exhibited outstanding catalytic activity for the activation of PMS toward selective oxidation of diethyl 1,4-dihydro-2,6-dimethyl-3,5-pyridinedicarboxylate(1,4-DHP)into diethyl2,6-dimethylpyridine-3,5-dicarboxylate,which serves as a valuable intermediate in the synthesis of various pharmaceutical compounds.Comprehensive experimental and characterization investigations verified that the nitrogen sites and defects are the primary active sites for PMS activation and selective oxidation of 1,4-DHP.This work offered an efficient approach for the fabrication of high-nitrogen-loading carbon materials for catalytic oxidation reactions.

Increase in the variability of terrestrial carbon uptake in response to enhanced future ENSO modulation

El Niño-Southern Oscillation(ENSO)is a major driver of climate change in middle and low latitudes and thus strongly influences the terrestrial carbon cycle through land-air interaction.Both the ENSO modulation and carbon flux variability are projected to increase in the future,but their connection still needs further investigation.To investigate the impact of future ENSO modulation on carbon flux variability,this study used 10 CMIP6 earth system models to analyze ENSO modulation and carbon flux variability in middle and low latitudes,and their relationship,under different scenarios simulated by CMIP6 models.The results show a high consistency in the simulations,with both ENSO modulation and carbon flux variability showing an increasing trend in the future.The higher the emissions scenario,especially SSP5-8.5 compared to SSP2-4.5,the greater the increase in variability.Carbon flux variability in the middle and low latitudes under SSP2-4.5 increases by 30.9%compared to historical levels during 1951-2000,while under SSP5-8.5 it increases by 58.2%.Further analysis suggests that ENSO influences mid-and low-latitude carbon flux variability primarily through temperature.This occurrence may potentially be attributed to the increased responsiveness of gross primary productivity towards regional temperature fluctuations,combined with the intensified influence of ENSO on land surface temperatures.

Construction of 3D porous Cu_(1.81)S/nitrogen-doped carbon frameworks for ultrafast and long-cycle life sodium-ion storage

Transition metal sulfides have great potential as anode mterials for sodium-ion batteries(SIBs)due to their high theoretical specific capacities.However,the inferior intrinsic conductivity and large volume variation during sodiation-desodiation processes seriously affect its high-rate and long-cyde performance,unbeneficial for the application as fast-charging and long-cycling SIBs anode.Herein,the three-dimensional porous Cu_(1.81)S/nitrogen-doped carbon frameworks(Cu_(1.81)S/NC)are synthesized by the simple and facile sol-gel and annealing processes,which can accommodate the volumetric expansion of Cu_(1.81)S nanoparticles and accelerate the transmission of ions and electrons during Na^(+)insertion/extraction processes,exhibiting the excellent rate capability(250.6 mA·g^(-1)at 20.0 A·g^(-1))and outstanding cycling stability(70% capacity retention for 6000 cycles at 10.0 A·g^(-1))for SIBs.Moreover,the Na-ion full cells coupled with Na_(3)V_(2)(PO_(4))_(3)/C cathode also demonstrate the satisfactory reversible specific capacity of 330.5 mAh·g^(-1)at 5.0 A·g^(-1)and long-cycle performance with the 86.9% capacity retention at 2.0 A·g^(-1)after 750 cycles.This work proposes a promising way for the conversionbased metal sulfides for the applications as fast-charging sodium-ion battery anode.

Preparation of Co/S co-doped carbon catalysts for excellent methylene blue degradation

S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.

Structural and microwave absorption properties of CoFe_(2)O_(4)/residual carbon composites

Electromagnetic interference,which necessitates the rapid advancement of substances with exceptional capabilities for bsorbing electromagnetic waves,is of urgent concern in contemporary society.In this work,CoFe_(2)O_(4)/residual carbon from coal gasification fine slag(CFO/RC)composites were created using a novel hydrothermal method.Various mechanisms for microwave absorption,including conductive loss,natural resonance,interfacial dipole polarization,and magnetic flux loss,are involved in these composites.Consequently,compared with pure residual carbon materials,this composite offers superior capabilities in microwave absorption.At 7.76GHz,the CFO/RC-2 composite achieves an impressive minimum reflection loss(RL_(min))of-43.99 dB with a thickness of 2.44 mm.Moreover,CFO/RC-3 demonstrates an effective absorption bandwidth(EAB)of up to 4.16 GHz,accompanied by a thickness of 1.18mm.This study revealed the remarkable capability of the composite to diminish electromagnetic waves,providing a new generation method for microwave absorbing materials of superior quality.

Covalent interfacial coupling of vanadium nitride with nitrogen-rich carbon textile boosting its lithium storage performance as binder-free anode

Eliminating the usage of metal current collectors and binders in traditional battery electrode configuration is an effective strategy to significantly improve the capacities of lithium ion batteries (LIBs). Herein, we demonstrate the construction of porous vanadium nitride (VN) nanosheet network in situ grown on nitrogen-rich (N-rich) carbon textile (N-C@P-VN) as lightweight and binder-free anode for LIBs. The N-rich carbon textile is used both as the current collector and host to store Li^(+), thus improving the specific capacities of binder-free VN anode and meanwhile reducing the inert mass of the whole cell. Moreover, the open spaces in carbon textile and vertically aligned pores in VN nanosheet network can not only provide an expressway for Li+ and e− transport, but also afford more active sites. As a result, the binder-free N-C@P-VN anode maintains a specific capacity of 1,040 mAh·g^(−1) (or an areal capacity of 2.6 mAh·cm^(−2)) after 100 cycles at 0.1 mA·cm^(−2) in half cell. Moreover, in an assembled N-C@P-VN//LiFePO4 full cell, it exhibits an areal capacity of 1.7 mAh·cm^(−2) after 300 cycles at 0.1 C. The synergistic strategy of N-C substrate and porous VN network could be applied to guide rational design of similar N-C@nitride or sulfide hybrid systems with corresponding sulfur-doped carbon textile as the substrate.

Perforated nitrogen-rich graphene-like carbon nanolayers supported Cu-In catalyst for boosting CO_(2) electroreduction to CO

The combination of a powerful CO_(2)-enriching carrier and robust active component provides a new idea for the construction of efficient catalysts for electrocatalytic CO_(2)reduction.Herein,novel perforated nitrogen-rich graphene-like carbon nanolayers(PNGC)are prepared from biomass derivatives,which promotes the oriented deposition of In-doped Cu_(2)(OH)_(3)(NO_(3))nanosheet patches.A robust Cu-In/PNGC composite catalyst is then obtained via simple in-situ electrochemical reduction.Unsurprisingly,CuIn/PNGC exhibits a CO Faradaic efficiency(FECO)of 91.3%and a remarkable CO partial current density(jCO)of 136.4 m A cm^(-2)at a moderate overpotential of 0.59 V for electrocatalytic CO_(2)reduction reaction(CO_(2)RR).DFT calculations and experimental studies indicate that the strong carrier effect of PNGC makes PNGC carried Cu-In nanosheets improved the adsorption capacity of CO_(2)gas,reconfigured electronic structure,and reduced free energy of key intermediate formation,thereby the CO_(2)activation and conversion are promoted.

Nitrogen-rich hierarchically porous carbon foams as high-performance electrodes for lithium-based dual-ion capacitor

Nitrogen-rich porous carbonaceous materials have shown great potential in energy storage and conversion applications due to their facile fabrication,high electronic conductivity,and improved hydrophilic property.Herein,three-dimensional porous N-rich carbon foams are fabricated through a one-step carbonization-activation method of the commercial melamine foam,and displaying hierarchically porous structure(macro-,meso-,and micro-pores),large surface area(1686.5 m2 g^-1),high N-containing level(3.3 at%),and excellent compressibility.The as-prepared carbon foams as electrodes for quasi-solid-state supercapacitors exhibit enhanced energy storage ability with 210 F g^-1 and 2.48c at 0.1 A g^-1,and150 F g^-1 and 1.77 F cm^-2 at 1 A g^-1,respectively.Moreover,as an electrode for lithium-based dual-ion capacitor,this distinctive porous carbon also delivers remarkable specific capacitance with 143.6 F g^-1 at0.1 A g^-1 and 116.2 F g^-1 at 1 A g^-1.The simple preparation method and the fascinating electrochemical performance endow the N-rich porous carbon foams great prospects as high-performance electrodes for electrochemical energy storage.

Nitrogen-rich carbon spheres made by a continuous spraying process for high-performance supercapacitors

Supercapacitors have high power densities, high efficiencies, and long cycling lifetimes; however, to enable their wider use, their energy densities must be significantly improved. The design and synthesis of improved carbon materials with better capacitance, rate performance, and cycling stability has emerged as the main theme of supercapacitor research. Herein, we report a facile synthetic method to prepare nitrogen-rich carbon particles based on a continuous aerosol- spraying process. The method yields particles that have high surface areas, a uniform microporous structure, and are highly N-doped, resulting in a synergism that enables the construction of supercapacitors with high energy and power density for use in both aqueous and commercial organic electrolytes. Furthermore, we have used density functional theory calculations to show that the improved performance is due to the enhanced wettability and ion adsorption interactions at the carbon/electrolyte interface that result from nitrogen doping. These findings provide new insights into the role of heteroatom doping in the capacitance enhancement of carbon materials; in addition, our method offers an efficient route for large-scale production of doped carbon.

Decoration of carbon encapsulated nitrogen-rich MoxN with few-layered MoSe2 nanosheets for high-performance sodium-ion storage

Transition metal nitrides have become the focus of research in sodium ion batteries(SIBs)due to their unique metal properties and high theoretical capacity.However,the low actual capacity is still the main bottleneck for their application.Herein,using Mo-aniline frameworks as precursors,the carbon encapsulated nitrogen-rich Mo_(x)N is decorated by few-layered MoSe_(2) nanosheets(MoSe_(2)@Mo_(x)N/C-I)after the facile calcinating,selenizing,and nitriding.The carbon encapsulation can effectively strengthen the structural stability of Mo_(x)N.The nitrogen-rich Mo_(x)N and decoration of few-layered MoSe_(2) can create rich heterointerfaces and extra active sites for rapid sodium-ion storage,thus promoting reaction kinetics and improving actual capacity.The MoSe_(2)@Mo_(x)N/C-I as an anode achieves a large reversible capacity of 522.8 mAh g^(-1)at 0.1 A g^(-1),and 254.3 mAh g^(-1)capacity is obtained after 6000 cycles at 5.0 A g^(-1),showing signally improved sodium-ion storage properties.The storage mechanisms and kinetic behaviors are described systematically via the advanced testing techniques and density functional theory(DFT)calculations.It is found that the nitrogen-rich Mo_(x)N as the substrate is the basis of long cycling stability,and the few-layered MoSe_(2) are the key to improving actual capacity.This work indicates that the decoration of few-layered selenides has a broad application prospect in high-performance metal-ion batteries.

Iron oxide encapsulated in nitrogen-rich carbon enabling high-performance lithium-ion capacitor

Lithium-ion capacitors(LICs)could combine the virtues of high power capability of conventional supercapacitors and high energy density of lithium-ion batteries.However,the lack of high-performance electrode materials and the kinetic imbalance between the positive and negative electrodes are the major challenge.In this study,Fe3O4 nanoparticles encapsulated in nitrogen-rich carbon(Fe3O4@NC)were prepared through a self-assembly of the colloidal Fe OOH with polyaniline(PANI)followed by pyrolysis.Due to the well-designed nanostructure,conductive nitrogen-rich carbon shells,abundant micropores and high specific surface area,Fe3O4@NC-700 delivers a high capacity,high rate capability and long cycling stability.Kinetic analyses of the redox reactions reveal the pseudocapacitive mechanism and the feasibility as negative material in LIC devices.A novel LIC was constructed with Fe3O4@NC-700 as the negative electrode and expanded graphene(EGN)as the positive electrode.The wellmatched two electrodes effectively alleviate the kinetic imbalance between the positive and negative electrodes.As a result,Fe3O4@NC-700//EGN LIC exhibits a wide operating voltage window,and thus achieves an ultrahigh energy density of 137.5 W h kg^-1.These results provide fundamental insights into the design of pseudocapacitive electrode and show future research directions towards the next generation energy storage devices.

Nitrogen-rich carbon nitrogen polymers for enhancing the sorption of uranyl

Nitrogen enrichment and increased nitrogen content is an effective strategy for enhancing adsorption of uranium by carbon nitride polymers.Herein,we reported the uranium absorption by using a structurally well-defined and nitrogen-rich carbon nitride polymer with C_(3)N_(5) stoichiometry for the first time.In comparison with the adsorption performance of g-C_(3)N_(4) for U(Ⅵ),the conjugation system of the material was increased by connecting the heptazine unit through the azo bridge in the structure of C_(3)N_(5),so that C_(3)N_(5) exhibited several times higher adsorption performance than that of g-C_(3)N_(4).The C_(3)N_(5) has high kinetics for uranyl ions,which can adsorb100 mg/g U(Ⅵ)in only 10 min and reach complete adsorption equilibrium in 60 min;the theoretical maximum adsorption capacity is 207 mg/g,meanwhile,the material exhibits high selectivity.The results of spectral analysis and theoretical calculations indicate that the process of uranyl ion capture by C3N5is a combination of physical and chemical adsorption,and its higher density of electronic states makes the electrostatic binding ability enhanced,which is favorable to the adsorption of uranyl ions by C_(3)N_(5).This work indicates that C_(3)N_(5) has great promise and application in the separation and enrichment of uranyl ions,and also provides a reference for the systematic investigation of the adsorption ability of nitrogenrich carbon nitrogen polymers on uranyl ions.

NiCoZn/C@melamine sponge-derived carbon composites with highperformance electromagnetic wave absorption

NiMZn/C@melamine sponge-derived carbon(MSDC)composites(M=Co,Fe,and Mn)were prepared by a vacuum pump-ing solution method followed by carbonization.A large number of carbon nanotubes(CNTs)homogeneously attached to the surfaces of the three-dimensional cross-linked of the sponge-derived carbon in the NiCoZn/C@MSDC composite,and CNTs were detected in the NiFeZn/C@MSDC and NiMnZn/C@MSDC composites.Ni_(3)ZnC_(0.7),Ni_(3)Fe,and MnO in-situ formed in the NiFeZn/C@MSDC and NiMnZn/C@MSDC composites.The CNTs in the NiCoZn/C@MSDC composite efficiently modulated its complex permittivity.Thus,the composite exhibited the best performance among the composites,with the minimum reflection loss(RL_(min))of-33.1 dB at 18 GHz and thickness of 1.4 mm.The bandwidth for RL of≤-10 dB was up to 5.04 GHz at the thickness of 1.7 mm and loading of 25wt%.The op-timized impedance matching,enhanced interfacial and dipole polarization,remarkable conduction loss,and multiple reflections and scat-tering of the incident microwaves improved the microwave absorption performance.The effects of Co,Ni,and Fe on the phase and mor-phology provided an alternative way for developing highly efficient and broadband microwave absorbers.

Prospects for green steelmaking technology with low carbon emissions in China

The steel industry is a major source of CO_(2) emissions,and thus,the mitigation of carbon emissions is the most pressing challenge in this sector.In this paper,international environmental governance in the steel industry is reviewed,and the current state of development of low-carbon technologies is discussed.Additionally,low-carbon pathways for the steel industry at the current time are proposed,emphasizing prevention and treatment strategies.Furthermore,the prospects of low-carbon technologies are explored from the perspective of transitioning the energy structure to a“carbon-electricity-hydrogen”relationship.Overall,steel enterprises should adopt hydrogen-rich metallurgical technologies that are compatible with current needs and process flows in the short term,based on the carbon substitution with hydrogen(prevention)and the CCU(CO_(2) capture and utilization)concepts(treatment).Additionally,the capture and utilization of CO_(2) for steelmaking,which can assist in achieving short-term emission reduction targets but is not a long-term solution,is discussed.In conclusion,in the long term,the carbon metallurgical process should be gradually supplanted by a hydrogen-electric synergistic approach,thus transforming the energy structure of existing steelmaking processes and attaining near-zero carbon emission steelmaking technology.

Construction and Application of a Regional Kilometer-Scale Carbon Source and Sink Assimilation Inversion System(CCMVS-R)

CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.

Absorption properties and mechanism of lightweight and broadband electromagnetic wave-absorbing porous carbon by the swelling treatment

Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.

Regulatable Orthotropic 3D Hybrid Continuous Carbon Networks for Efficient Bi-Directional Thermal Conduction

Vertically oriented carbon structures constructed from low-dimen-sional carbon materials are ideal frameworks for high-performance thermal inter-face materials(TIMs).However,improving the interfacial heat-transfer efficiency of vertically oriented carbon structures is a challenging task.Herein,an orthotropic three-dimensional(3D)hybrid carbon network(VSCG)is fabricated by depositing vertically aligned carbon nanotubes(VACNTs)on the surface of a horizontally oriented graphene film(HOGF).The interfacial interaction between the VACNTs and HOGF is then optimized through an annealing strategy.After regulating the orientation structure of the VACNTs and filling the VSCG with polydimethylsi-loxane(PDMS),VSCG/PDMS composites with excellent 3D thermal conductive properties are obtained.The highest in-plane and through-plane thermal conduc-tivities of the composites are 113.61 and 24.37 W m^(-1)K^(-1),respectively.The high contact area of HOGF and good compressibility of VACNTs imbue the VSCG/PDMS composite with low thermal resistance.In addition,the interfacial heat-transfer efficiency of VSCG/PDMS composite in the TIM performance was improved by 71.3%compared to that of a state-of-the-art thermal pad.This new structural design can potentially realize high-performance TIMs that meet the need for high thermal conductivity and low contact thermal resistance in interfacial heat-transfer processes.

Enhancing the Interaction of Carbon Nanotubes by Metal-Organic Decomposition with Improved Mechanical Strength and Ultra-Broadband EMI Shielding Performance

The remarkable properties of carbon nanotubes(CNTs)have led to promising applications in the field of electromagnetic inter-ference(EMI)shielding.However,for macroscopic CNT assemblies,such as CNT film,achieving high electrical and mechanical properties remains challenging,which heavily depends on the tube-tube interac-tions of CNTs.Herein,we develop a novel strategy based on metal-organic decomposition(MOD)to fabricate a flexible silver-carbon nanotube(Ag-CNT)film.The Ag particles are introduced in situ into the CNT film through annealing of MOD,leading to enhanced tube-tube interactions.As a result,the electrical conductivity of Ag-CNT film is up to 6.82×10^(5) S m^(-1),and the EMI shielding effectiveness of Ag-CNT film with a thickness of~7.8μm exceeds 66 dB in the ultra-broad frequency range(3-40 GHz).The tensile strength and Young’s modulus of Ag-CNT film increase from 30.09±3.14 to 76.06±6.20 MPa(~253%)and from 1.12±0.33 to 8.90±0.97 GPa(~795%),respectively.Moreover,the Ag-CNT film exhibits excellent near-field shield-ing performance,which can effectively block wireless transmission.This innovative approach provides an effective route to further apply macroscopic CNT assemblies to future portable and wearable electronic devices.