In Situ Atomic Reconstruction Engineering Modulating Graphene-Like MXene-Based Multifunctional Electromagnetic Devices Covering Multi-Spectrum

With the diversified development of big data,detection and precision guidance technologies,electromagnetic(EM)functional materials and devices serving multiple spectrums have become a hot topic.Exploring the multispectral response of materials is a challenging and meaningful scientific question.In this study,MXene/TiO_(2)hybrids with tunable conduction loss and polarization relaxation are fabricated by in situ atomic reconstruction engineering.More importantly,MXene/TiO_(2)hybrids exhibit adjustable spectral responses in the GHz,infrared and visible spectrums,and several EM devices are constructed based on this.An antenna array provides excellent EM energy harvesting in multiple microwave bands,with|S11|up to−63.2 dB,and can be tuned by the degree of bending.An ultra-wideband bandpass filter realizes a passband of about 5.4 GHz and effectively suppresses the transmission of EM signals in the stopband.An infrared stealth device has an emissivity of less than 0.2 in the infrared spectrum at wavelengths of 6-14μm.This work can provide new inspiration for the design and development of multifunctional,multi-spectrum EM devices.

Layer-Contacted Graphene-Like BN/Ultrathin Bi_(3)O_(4)Br Stacking for Boosting Photocatalytic Molecular Oxygen Activation

Novel graphene-like boron nitride(BN)/Bi_(3)O_(4)Br photocatalysts have been controllably synthesized through a facile solvothermal method for the first time. Layer contact stacking between graphene-like BN and ultrathin Bi_(3)O_(4)Br was achieved with strong interaction. Dehalogenation is designed to harvest more visible light, and the ultrathin structure of Bi_(3)O_(4)Br is designed to accelerate charge transfer from inside to the surface. After graphene-like BN was engineered, photocatalytic performance greatly improved under visible light irradiation. Graphene-like BN can act as a surface electron-withdrawing center and adsorption center, facilitating molecular oxygen activation. O_(2)^(·-)was determined to be the main active species during the degradation process through analyses of electron spin resonance and XPS valence band spectra.

Flexible free-standing graphene-like film electrode for supercapacitors by electrophoretic deposition and electrochemical reduction

Electrophoretic deposition in conjunction with electrochemical reduction was used to make flexible free-standing graphene-like films. Firstly, graphene oxide （GO） film was deposited on graphite substrate by electrophoretic deposition method, and then reduced by subsequent electrochemical reduction of GO to obtain reduced GO （ERGO） film with high electrochemical performance. The morphology, structure and electrochemical performance of the prepared graphene-like film were confirmed by SEM, XRD and FT-IR. These unique materials were found to provide high specific capacitance and good cycling stability. The high specific capacitance of 254 F/g was obtained from cyclic voltammetry measurement at a scan rate of 10 mV/s. When the current density increased to 83.3 A/g, the specific capacitance values still remained 132 F/g. Meanwhile, the high powder density of 39.1 kW/kg was measured at energy density of 11.8 W-h/kg in 1 mol/L H2SO4 solution. Furthermore, at a constant scan rate of 50 mV/s, 97.02% of its capacitance was retained for 1000 cycles. These promising results were attributed to the unique assembly structure of graphene film and low contact resistance, which indicated their potential application to electrochemical capacitors.

Facile Synthesis of N-Doped Graphene-Like Carbon Nanoflakes as Efficient and Stable Electrocatalysts for the Oxygen Reduction Reaction

A series of N-doped carbon materials(NCs)were synthesized by using biomass citric acid and dicyandiamide as renewable raw materials via a facile onestep pyrolysis method. The characterization of microstructural features shows that the NCs samples are composed of few-layered graphene-like nanoflakes with controlled in situ N doping, which is attributed to the confined pyrolysis of citric acid within the interlayers of the dicyandiamide-derived g-C_3N_4 with high nitrogen contents. Evidently, the pore volumes of the NCs increased with the increasing content of dicyandiamide in the precursor. Among these samples, the NCs nanoflakes prepared with the citric acid/dicyandiamide mass ratio of 1:6, NC-6,show the highest N content of ~6.2 at%, in which pyridinic and graphitic N groups are predominant. Compared to the commercial Pt/C catalyst, the as-prepared NC-6 exhibits a small negative shift of ~66 mV at the half-wave potential, demonstrating excellent electrocatalytic activity in the oxygen reduction reaction. Moreover, NC-6 also shows better long-term stability and resistance to methanol crossover compared to Pt/C. The efficient and stable performance are attributed to the graphene-like microstructure and high content of pyridinic and graphitic doped nitrogen in the sample, which creates more active sites as well as facilitating charge transfer due to the close four-electron reaction pathway. The superior electrocatalytic activity coupled with the facile synthetic method presents a new pathway to cost-effective electrocatalysts for practical fuel cells or metal–air batteries.

Triple-phase interfaces of graphene-like carbon clusters on antimony trisulfide nanowires enable high-loading and long-lasting liquid Li_(2)S_(6)-based lithium-sulfur batteries

High performance of lithium-sulfur batteries have been dragged down by their shuttling behavior which is complicated multiphase transition-based 16-electron redox reactions of the S8/Li2 S.In this article,the triple-phase interfaces of graphene-like carbon clusters on antimony trisulfide(C-Sb_(2)S_(3))nanowires are tailored to design a multifunctional polysulfide host which can inhibit migration of polysulfides and accelerate conversion kinetics of redox electrochemical reactions.Benefiting from the triple-interface design of polysulfides/Sb_(2)S_(3)/carbon clusters,the C-Sb_(2)S_(3) electrode not only anchors polysulfide migration by the synergistic effect of Sb,S,and C atoms as interfacial active sites,but also the graphene-like carbon clusters shorten the diffusion paths to further favor redox electron/ion transport through the liquid(electrolyte/polysulfide)and solid(Li2 S/S8,carbon clusters,and Sb_(2)S_(3))-based triple-phases.Therefore,these Li_(2)S_(6)-based C-Sb_(2)S_(3) cells possess high sulfur loading,excellent cycling stability,impressive specific capacity,and great rate capability.This work of interfacial engineering reveals insight for powering reaction kinetics in the complicated multistep catalysis reaction with multiphase evolution-based chargetransfer/non-transfer processes.

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.

Adsorptions of metal adatoms on graphene-like BC3 and their rich electronic properties： A first-principles study

Density functional calculations have been performed to investigate the adsorption of twenty two different kinds of metal adatoms on graphene-like BC3. In contrast to the graphene adsorbed with adatoms, the BC3 with adatoms shows many interesting properties.（1） The interaction between the metal adatoms and the BC3 sheet is remarkably strong. The Li, Na, K, and Ca possess the binding energies larger than the cohesive energies of their corresponding bulk metals.（2）The Li, Na, and K adatoms form approximately ideal ionic bonds with BC3, while the Be, Mg, and Ca adatoms form ionic bonds with BC3 with slight hybridization of covalent bonds. The Al, Ga, In, Sn, and all transition metal adatoms form covalent bonds with BC3.（3） For all the structures studied, there exhibit metal, half-metal, semiconducting, and spin-semiconducting behaviors. Especially, the BC3 with Co adatom shows a quantum anomalous Hall（QAH） phase with a Chern number of -1 based on local density approximation calculations.（4） For Li, Na, K, Ca, Ga, In, Sn, Ti, V, Cr,Ni, Pd, and Pt, there exists a trend that the adatom species with lower ionization potential have lower work function. Our results indicate the potential applications of functionalization of BC3 with metal adatoms.

Compensation temperatures and hysteresis behaviors of a graphene-like trilayer

This work focuses on the ground-state phase diagram,the compensation temperatures and the critical behaviors of a ferrimagnetic graphene-like trilayer induced by crystal fields and exchange couplings.The simulation results show that a negative decrease in crystal field or an increase in exchange coupling can increase the critical temperature.More importantly,an M curve with double compensation temperatures can be observed,which is not predicted by the Neel theory.This remarkable compensation phenomenon has potential application value in the field of magnetic recording.

Compensation temperature and hysteresis behaviors of a graphene-like bilayer:Monte Carlo Study

Using the Monte Carlo method,the compensation temperature and hysteresis loops of a ferrimagnetic mixed spin-3/2 and spin-5/2 Ising-type graphene-like bilayer are investigated induced by different physical parameters such as crystal field,exchange coupling,external magnetic field,and temperature.The variations of magnetization,magnetic susceptibility,specific heat,and internal energy with the change of temperature are discussed.In addition,we also plot the phase diagrams including transition temperature and compensation temperature.Finally,multiple hysteresis loops under certain parameters are given.

Enhancing kinetics of Li-S batteries by graphene-like N,S-codoped biochar fabricated in NaCl non-aqueous ionic liquid

Graphene-like N,S-codoped bio-carbon nanosheets(GNSCS) were prepared by a facile and environment-friendly NaCl non-aqueous ionic liquid route to house sulfur for lithium-sulfur battery. The natural nori powder was calcined at 900°C for 3 h under Ar, in which NaCl non-aqueous ionic liquid can exfoliate carbon aggregates into nanosheets. The structural characterization of GNSCS by a series of techniques demonstrates the graphene-like feature.When evaluated as the matrix for sulfur cathode, GNSCS/S exhibits more prominent cycling stability and rate capability.A discharge capacity of 548 mA h g-1 at a current density of 1.6 A g-1 after 400 cycles was delivered with a capacity fade rate of only 0.13% per cycle and an initial Coulombic efficiency(CE) as high as 99.7%. When increasing the areal sulfur loading up to 3 mg cm-2, the discharge capacity can still be retained at 647 mA h g-1 after more than 100 cycles with a low capacity degradation of only ~0.30% per cycle. The features of N/S dual-doping and the graphene-like structure are propitious to the electron transportation, lithium-ion diffusion and more active sites for chemically adsorbing polysulfides. It is anticipated that other functional biochar carbon can also be attained via the low-cost, sustainable and green method.

Co/N co-doped graphene-like nanocarbon for highly efficient oxygen reduction electrocatalyst

The development of efficient and inexpensive graphene-based electrocatalysts is of great significance to promote the commercial application of fuel cell and metal-air batteries. In this paper, a new type of Co and N co-doped graphene-like nanocarbon(Co/N-GLC) material was prepared by nano-silicon protection and high temperature pyrolysis.The obtained Co/N-GLC catalyst not only has a similar morphology of graphene, but also possesses a high specific surface area(809 m2 g-1) with hierarchical porous structure(micropores/mesopores), and relative high active dopants content.These properties endow it with a good oxygen reduction activity in alkaline media, which can be comparable to commercial Pt/C catalyst. Moreover, the assembled zinc-air batteries using Co/N-GLC catalyst as the air electrode display a better discharge performance and higher stability compared to that of Pt/C electrode. This work demonstrates that the prepared graphene-like carbon catalyst has a good prospect,which can replace noble metal catalyst at the cathode in metalair batteries.

From graphite to porous graphene-like nanosheets for high rate lithium-ion batteries

Graphene nanosheets possess a promising potential as electrodes in Li-ion batteries （LIBs）; consequently, the development of low-cost and high-productivity synthetic approaches is crudal. Herein, porous grapheneqike nanosheets （PGSs） have been synthesized from expandable graphite （EG） by initially intercalating phosphoric acid, and then performing annealing to enlarge the interlayer distance of EG, thus fadlitating the successive intercalation of zinc chloride. Subsequently, the following pyrolysis of zinc chloride in the EG interlayer promoted the formation of the porous PGS structure; meanwhile, the gas produced during the formation of the porous structure could exfoliate the EG to graphene-like nanosheets. The synthetic PGS material used as LIB anode exhibited superior Li＋ storage performance, showing a remarkable discharge capacity of 830.4 mAh.g-1 at 100 mA.g-1, excellent rate capadty of 211.6 mAh＇g-1 at 20,000 mA-g-1, and excellent cycle performance （near 100% capacity retention after 10,000 cycles）. The excellent rate performance is attributed to the Li＋ ion rapid transport in porous structures and the high electrical conductivity of graphene-like nanosheets. It is expected that PGS may be widely used as anode material for high-rate LIBs via this facile and low-cost route by employing EG as the raw material.

Analysis of graphene-like activated carbon derived from rice straw for application in supercapacitor

Activated carbons with large surface area, abundant microporosity and low cost are the most commonly used electrode materials for energy storage devices. However, activated carbons are conventionally made from fossil precursors, such as coal and petroleum, which are limited resources and easily aggregate large block in high temperature carbonization processes. In this novel work, we examined the use of rice straw as a potential alternative carbon source precursor for the production of graphene-like active carbon. A very slack activated carbon with ultra-thin two-dimensional （2D） layer structure was prepared by our proposed approach in this work, which includes a pre-treatment process and potassium hydroxide activation at high temperatures. The obtained active carbon derived from rice straw exhibited a capacitance of 255 Fig at 0.5 A/g, excellent rate capability, and long cycling capability （98% after 10,000 cycles）.

Design of graphene-like gallium nitride and WS_2/WSe_2 nanocomposites for photocatalyst applications

The geometric,electronic and optical properties of the graphene-like gallium nitride(GaN) monolayer paired with WS_2 or WSe_2 were studied systematically using the first-principles calculations.GaN interacts with WS2 or WSe_2 via van der Waals interaction and all the most stable configurations of these two nanocomposites exhibit direct band gap characteristics.Meanwhile,the type-Ⅱ heterojunctions are formed because the conduction band minimums and valence band maximums are respectively contributed by WS_2(or WSe_2) and GaN.The imaginary parts of the dielectric function and the absorption spectra of the heterostructures were also calculated and the relatively improved optical properties were observed because of the new interband transitions.In addition,the band offsets as well as the intrinsic electric fields resulting from the interlayer charge transfer indicate that the electron-hole pairs recombination can be effectively inhibited,which is conducive for the photocatalysis process.Moreover,the band gaps of the heterostructures can be modulated by applying biaxial strains and even shift away the conduction band edge potential from the H^+/H_2potential in a certain range,which further enhances the photocatalyst performance.The results indicate that GaN/WS2 or GaN/WSe_2 nanocomposites are good candidate materials for photocatalyst or photoelectronic applications.

Graphene-like h-BN supported polyhedral NiS_(2)/NiS nanocrystals with excellent photocatalytic performance for removing rhodamine B and Cr(Ⅵ)

Human health is deteriorating due to the effluent containing heavy metal ions and organic dyes.Hence,photoreduction of Cr(Ⅵ)to Cr(Ⅲ)and degradation of rhodamine B(RhB)using a novel photocatalyst is particularly important.In this work,h-BN/NiS_(2)/NiS composites were prepared via a simple solvothermal method and a double Z-scheme heterojunction was constructed for efficiently removing RhB and Cr(Ⅵ).The 7 wt-%h-BN/NiS_(2)/NiS composites were characterized via a larger specific surface area(15.12 m^(2)·g^(−1)),stronger light absorption capacity,excellent chemical stability,and high yield of electrons and holes.The experimental result indicated that the photoreduction efficiency of the 7 wt-%h-BN/NiS_(2)/NiS photocatalyst achieved 98.5%for Cr(Ⅵ)after 120 min,which was about 3 times higher than that of NiS_(2)/NiS(34%).However,the removal rate of RhB by the 7 wt-%h-BN/NiS_(2)/NiS photocatalyst reached 80%.This is due to the double Z-scheme heterojunction formed between NiS_(2)/NiS and h-BN,which improved the charge separation efficiency and transmission efficiency.Besides,the influence of diverse photogenerated electron and hole scavengers upon the photoreduction of Cr(Ⅵ)was studied,the results indicated that graphene-like h-BN promoted transportation of photoinduced charges on the surface of the h-BN/NiS_(2)/NiS photocatalyst via the interfacial effects.

Photocatalytic water splitting of ternary graphene-like photocatalyst for the photocatalytic hydrogen production

In recent times,there has been an increasing demand for energy which has resulted in an increased consumption of fossil fuels thereby posing a number of challenges to the environment.In the course finding possible solutions to this environmental canker,solar photocatalytic water splitting to produce hydrogen gas has been identified as one of the most promising methods for generating renewable energy.To retard the recombination of photogenerated carriers and improve the efficiency of photocatalysis,the present paper reports a facile method called the hydrothermal method,which wa s used to prepare ternary graphene-like photocatalyst.A“Design Expert”was used to investigate the influence of the loading weight of Mo and GO as well as the temperature of hydrothermal reaction and their interactions on the evolution of hydrogen(H 2)in 4 h.The experimental results showed that the ternary graphene-like photocatalyst has a strong photocatalytic hydrogen production activity compared to that of pure SiC.In particular,the catalyst added 2.5 wt%of GO weight yielded the highest quantum of 21.69%at 400-700 nm of wavelength.The optimal evolution H2 in 4 h conditions was obtained as follows:The loading weight of Mo was 8.19 wt%,the loading weight of GO was 2.02 wt%,the temperature of the hydrothermal reaction was 200.93℃.Under the optimum conditions,the evolution of H2 in 4h could reach 4.2030 mL.

Oxidation layering mechanism of graphene-like MoS2 prepared by the intercalation-detonation method

Graphene-like MoS2 has attracted significant interest because of its unique electronic, optical, and catalytic properties with two-dimensional lamellar structure. Three kinds of intercalated MoS2 samples were prepared using different oxidation layering methods, which are the first steps of intercalation-detonation. The oxidation layering mechanism of graphene-like MoS2 was systematically characterized using Fourier transform infrared, X-ray photoelectron, and Raman spectroscopy techniques. The bulk MoS2 sample was gradually oxidized from the edge to the interlayer in the presence of concentrated H2SO4 and KMnO4. A large number of hydroxyl groups were bonded to the sulfur atom layer, forming S-OH bonds in the basal planes of the MoS2 structure. The addition of deionized water to concentrated H2SO4 generated a large amount of heat, promoting the generation of more S-OH bonds, destroying residual Van der Waals forces between the layers, and finally stripping off parts of the flakes. The continuous addition of deionized water in the high temperature stage resulted in the largest oxidative intercalation effect. Additional136 the I/factor was determined to compare the intensities of Blu and Alg peaks in the Raman spectra and quantify the effect of oxidative intercalation. The highest value of q was obtained when deionized water was added continuously during the preparation of intercalated MoS2.

Dynamic magnetic properties of Ising graphene-like monolayer

Dynamic magnetic properties of the mixed-spin(3/2,5/2)Ising graphene-like monolayer in an oscillating magnetic field are studied by means of Monte Carlo simulation.The effects of Hamiltonian parameters such as crystal field and time-dependent oscillating magnetic field on the dynamic order parameter,susceptibility and internal energy of the system are well presented and explained.Moreover,much attention has also been dedicated to the phase diagrams with different parameters in order to better comprehend the impacts of these parameters on the critical temperature.Our results reveal that the crystal fields of two sublattices have similar effects on the critical temperature,but the bias field and amplitude of oscillating field have opposite effects on it.We hope that our research can be of guiding significance to the theoretical and experimental studies of graphene-like monolayer.

High energy superstable hybrid capacitor with a self-regulated Zn/electrolyte interface and 3D graphene-like carbon cathode

Rechargeable aqueous zinc ion hybrid capacitors(ZIHCs),as an up-and-comer aqueous electrochemical energy storage system,endure in their infancy because of the substandard reversibility of Zn anodes,structural deterioration of cathode materials,and narrow electrochemical stability window.Herein,a scalable approach is described that addresses Zn-anode/electrolyte interface and cathode materials associated deficiencies and boosts the electrochemical properties of ZIHCs.The Zn-anode/electrolyte interface is self-regulated by alteration of the traditional Zn2+electrolyte with Na-based supporting salt without surrendering the cost,safety,and green features of the Zn-based system which further validates the excellent reversibility over 1100 h with suppressed hydrogen evolution.The deficits of cathode materials were overcome by using a high-mass loaded,oxygen-rich,3D,multiscaled graphene-like carbon(3D MGC)cathode.Due to the multiscaled texture,high electronic conductivity,and oxygen-rich functional groups of 3D MGC,reversible redox capacitance was obtained with a traditional adsorption/desorption mechanism.Prototype ZIHCs containing the modified electrolyte and an oxygen-rich 3D MGC cathode resulted in battery-like specific energy(203 Wh kg1 at 1.6 A g^(-1))and supercapacitor-type power capability(4.9 kW kg1 at 8 A g^(-1))with outstanding cycling durability(96.75%retention over 30000 cycles at 10 A g^(-1)).These findings pave the way toward the utilization of highly efficient ZIHCs for practical applications.

Double-sided surface functionalization: An effective approach to stabilize and modulate the electronic structure of graphene-like borophene

Graphene-like borophene was theoretically proposed and recently synthesized on Al(111)surface,however,how to conquer its structural instability is still an open question.By means of density functional theory computations,we theoretically predicted that honeycomb borophene can be well stabilized by double-sided surface passivation with monovalent functional groups(X=F,Cl,Br,I,OH,and NH2)due to the electron redistributions.The system undergoes the transition from metallic to semiconducting upon functionalization,while the energy gap depends on the choice of functional groups.Under external strain,the gap values can be manipulated over a broad range.Our further calculations indicated that the functionalized borophene possesses moderate and anisotropic carrier mobility,which is comparable to or even higher than some 2D materials such as MoS2 and phosphorene.Our work provides a feasible strategy to effectively stabilize the graphene-like borophene and tune the electronic properties with great potentials for electronic applications.