Review:Layer⁃Number Controllable Preparation of High⁃Quality Graphene for Wide Applications

Graphene, a well-known two-dimensional(2 D) material, has sparked broad enthusiasm in both scientific and industrial communities in these years, due to its exceptional electrical, thermal, mechanical, and versatile properties. However, many properties and applications of graphene are layer-number dependent. The preparation of high-quality graphene with controlled layer numbers is full of challenge, since the layer number varies much with the synthesis routes and relevant experimental conditions. Hence, there is an urgent need to improve the layer-number controllability of graphene preparation. Generally, graphene can be prepared by two complementary approaches: "top-down" and "bottom-up". Since they have their own advantages, the recent advances in the layer-number tunable preparation of high-quality graphene are separately studied from the two aspects in this review, especially those dedicated to single parameter. Some effective strategies are discussed in detail, mainly including 1) supercritical-CO2 assisted sonication, electrochemical exfoliation of graphite intercalation compounds, and layer-by-layer thinning with plasma or laser, for "top-down" graphene;2) chemical vapor deposition(CVD) on dual-metal substrate, ion-implantation CVD, layer-by-layer CVD, plasma-enhanced CVD, layered-double-hydroxides template-assisted CVD;and 3) graphite-enclosure assisted epitaxial growth and pulsed-magnetron-sputtering assisted physical vapor deposition for "bottom-up" graphene on various substrates. In addition, the respective advantages of graphene with different layer numbers in properties and applications are also presented. Finally, the contribution concludes with some important perspectives on the remained challenges and future perspectives.

Efficient Preparation and Characterization of Functional Graphene with Versatile Applicability

Graphene,as star versatile materials having extraordinarily high electric conductivity,electron mobility,thermal conductivity,thermal stability,optical transparency,and mechanical strength,has attracted much attention from scientists and engineers in the field of materials,chemistry,physics,energy,and environment in the last decade and achieved fruitful accomplishment.This review discusses preparation strategies,functionality,characterization,and applications for two dimensional nanosheet and quasi-onedimensional nanoribbon of graphene through direct exfoliation of graphite,chemical vapor deposition of hydrocarbon,laser-induced direct synthesis of graphene,laser etched graphene oxide in the dry state without the use of toxic reducing agent hydrazine,unzipping carbon nanotube,and polycondensation of polycyclic aromatics on the basis of 178 representative references mostly in 2015.The stabilization of graphene oxide prepared in chemical preparation in " top-down" is emphasized.Several vital classic methods of characterizing molecular structure,C/O ratio,defect,morphology,single-or few-layered( 2 to 10 layers) structure,porous and hollow structures,including Raman spectroscopy,AFM,SEM,TEM,STM,electron diffraction,X-ray diffraction,and X-ray photoelectron spectroscopy are systematically introduced.Because graphene possesses novel incomparable multifunctionalities,its versatile applications as novel conducting additives,reinforcing filler,separation membrane,sensor,anticorrosive coating,catalyst,electromagnetic shield,lubricant,and flexible electrode materials in electrochemical and electronic devices,including photovoltaic cells,supercapacitors,rechargeable batteries,sensors,field effect transistors,light emitting diodes,separation membranes,adsorbents and absorbents,catalysts,electro-optic modulator,terahertz emitter and detector,and semiconductors,have been mentioned.Especially in the aspect of both high performance and cost-effectiveness,graphene is expected to be even superior to the expensive carbon nanotubes.

Effect of preparation methods on the adsorption property of municipal solid waste-based carbon materials

Three different preparation methods including steam physical activation, catalytic carbonation and KOH chemical activation methods were used to prepare municipal solid waste- based carbon materials. The methylene blue （MB） adsorption value was applied to evaluate the adsorption capabilities of the prepared carbon materials. The effects of preparation methods on adsorption capability and yield of products were investigated. The yield of carbon materials with the catalytic carbonation method is the highest, and the KOH activation method is the second level. Considering the adsorption performance, the KOH activation method is much more favorable. Among the different components of municipal solid waste-based carbon materials, the adsorption properties of the single component of paperboard, the double components of tire and paperboard, the triple components of tire, paperboard and polyvinyl chloride （PVC）, and the multi-component mixtures are better than those of other single-, double-, triple- and multi-component mixtures, respectively.

Effect of preparation methods on the structure and catalytic performance of Fe–Zn/K catalysts for CO2 hydrogenation to light olefins

Potassium promoted iron–zinc catalysts prepared by co-precipitation method(C–Fe–Zn/K),solvothermal method(S–Fe–Zn/K)and hydrothermal method(H–Fe–Zn/K)could selectively convert CO_2to light olefins,respectively.The physicochemical properties of the obtained catalysts were determined by SEM,N_2physisorption,XRD,H_2-TPR,CO_2-TPD and XPS measurements.The results demonstrated that preparation methods had great influences on the morphology,phase structures,reduction and adsorption behavior,and hence the catalytic performance of the catalysts.The samples prepared by hydrothermal and co-precipitation method generated small uniform particles and led to lower specific surface area.In contrast,microspheres with larger specific surface area were formed by self-assembly of nanosheets using solvothermal method.ZnFe_2O_4was the only detectable phase in the fresh C–2Fe–1Zn/K,S–3Fe–1Zn/K and S–2Fe–1Zn/K samples.ZnFe_2O_4and ZnO co-existed with increasing Zncontent in S–1Fe–1Zn/K sample,while ZnO and Fe_2O_3could be observed over H–2Fe–1Zn/K sample.All the used samples contained Fe_3O_4,ZnO and Fe_5C_2.The peak intensity of ZnO was strong in the AR-H–2Fe–1Zn/K sample while it was the lowest in the AR-C–2Fe–1Zn/K sample after reaction.The formation of ZnFe_2O_4increased the interaction between iron and zinc for C–2Fe–1Zn/K and S–Fe–Zn/K samples,causing easier reduction of Fe_2O_3to Fe_3O_4.The surface basicity of the sample prepared by co-precipitation method was much more than that of the other two methods.During CO_2hydrogenation,all the catalysts showed good activity and olefin selectivity.The CO selectivity was increased with increasing Zncontent over S–Fe–Zn/K samples.H–2Fe–1Zn/K catalyst preferred to the production of C_5^+hydrocarbons.CO_2conversion of 54.76%and C_2~=–C_4~=contents of 57.38%were obtained on C–2Fe–1Zn/K sample,respectively.

Preparation and capacitance properties of Ni foam@graphene@Co_(3)O_(4)composite electrode materials

Graphene under high temperature was prepared and loaded on Ni foam.Then,cobalt tetroxide precursor was grown on Ni foam in situ by the hydrothermal method.Finally,the sample was burned at high temperature to obtain Co_(3)O_(4)+graphene@Ni.The hydrothermal method used in this paper is easy to operate,with low-risk factors and environmental protection.The prepared Co_(3)O_(4)+graphene@Ni electrode exhibits superior electrochemical performance than Co_(3)O_(4)@Ni electrode.At a current density of 1 A/g,the specific capacitance of the Co_(3)O_(4)+graphene@Ni electrode calculated by a charge-discharge test is 935 F/g,which is much larger than that of Co_(3)O_(4)@Ni electrode of 340 F/g.

Three-dimensional oxygen-doped porous graphene:Sodium chloridetemplate preparation,structural characterization and supercapacitor performances

Supercapacitor is a new type of energy storage device,which has the advantages of high-power property and long cycle life.In this study,three-dimensional graphene(3 D-GN)with oxygen doping and porous structure was prepared from graphene oxide(GO)by an inexpensive sodium chloride(NaCl)template,as a promising electrode material for the supercapacitor.The structure,morphology,specific surface area,pore size,of the sample were characterized by XRD,SEM,TEM and BET techniques.The electrochemical performances of the sample were tested by CV and CDC techniques.The 3 D-GE product is a threedimensional nano material with hierarchical porous structures,its specific surface area is much larger than that of routine stacked graphene(GN),and it contains a large number of mesoporous and macropores,a small amount of micropores.The capacitance characteristics of the 3 D-GN electrode material are excellent,showing high specific capacitance(173.5 F·g^(-1)at 1 A·g^(-1)),good rate performance(109.2 F·g^(-1)at 8 A·g^(-1))and long cycle life(88%capacitance retention after 10,000 cycles at 8 A·g^(-1))

Preparation of Graphene Materials and Their Applications in the Field of Electrochemistry

In the development of modern society, many new materials and technologies have been integrated into the development of various industries. As a new type of two-dimensional carbon nanomaterials, graphene has great advantages in physical and chemical properties and is widely used in various fields of development. Among them, the electrochemical method is one of the important ways to prepare graphene materials, which has the characteristics of quickness and environmental protection, and can effectively produce a large amount of high-quality graphene and its composite materials. Based on this, the paper introduces the preparation method of graphene materials and studies the application of graphene materials in the field of electrochemistry.

Influence of preparation methods on CuO-CeO_2 catalysts in the preferential oxidation of CO in excess hydrogen

Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen （PROX） over CuO-CeO2 catalysts has been investigated and CuO-CeO2 catalysts are characterized using BET, XPS, XRD, UV Raman, and TPR techniques. The results show that the catalysts prepared by coprecipitation have smaller particle sizes, well-dispersed CuOx species, more oxygen vacancies, and are more active in the PROX than those prepared by the other methods. However. the inverse coprecipitation depresses the catalytic performance of CuO-CeO2 catalysts and causes the growth of CuO-CeO2 because of different pH value in the precipitation process.

Effect of Preparation Methods of Bi_(2)O_(3) Nanoparticles on their Photocatalytic Activity

Bi 2O 3 nanoparticles were prepared by means of ammonia precipitation, polyol mediated methods and microemulsion chemical method. The structure and properties of the as-prepared nanoparticles, having been submitted to a heat-treatment test at 750 ℃, were characterized by means of XRD, BET, XPS and UV-Vis absorption techniques. The photocatalytic oxidation reactions of benzene, toluene and xylene were used as the model reaction to measure the photocatalytic activity of Bi 2O 3 nanoparticles, respectively. The results show that the crystallite size of Bi 2O 3 prepared with different methods and calcined at 750 ℃ were 50.6, 38.5 and 31.5 nm, respectively. The photocatalytic activity of Bi 2O 3 nanoparticles prepared with the microemulsion chemical method was higher than that of the particles prepared with the polyol mediated method; and that of the particles prepared with the micromulsion chemical method was the highest among the three. The degradation rates of the three pollutants xylene, toluene and benzene decreased in sequence.

Influence of preparation methods on the physicochemical properties and catalytic performance of MnO_x-CeO_2 catalysts for NH_3-SCR at low temperature

This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature. Five different methods, namely, mechanical mixing, impregnation,hydrothermal treatment, co‐precipitation, and a sol‐gel technique, were used to synthesizeMnOx‐CeO2 catalysts. The catalysts were characterized in detail, and an NH3‐SCR model reaction waschosen to evaluate the catalytic performance. The results showed that the preparation methodsaffected the catalytic performance in the order: hydrothermal treatment > sol‐gel > co‐precipitation> impregnation > mechanical mixing. This order correlated with the surface Ce3+ and Mn4+ content,oxygen vacancies and surface adsorbed oxygen species concentration, and the amount of acidic sitesand acidic strength. This trend is related to redox interactions between MnOx and CeO2. The catalystformed by a hydrothermal treatment exhibited excellent physicochemical properties, optimal catalyticperformance, and good H2O resistance in NH3‐SCR reaction. This was attributed to incorporationof Mnn+ into the CeO2 lattice to form a uniform ceria‐based solid solution (containing Mn‐O‐Cestructures). Strengthening of the electronic interactions between MnOx and CeO2, driven by thehigh‐temperature and high‐pressure conditions during the hydrothermal treatment also improved the catalyst characteristics. Thus, the hydrothermal treatment method is an efficient and environment‐friendly route to synthesizing low‐temperature denitrification (deNOx) catalysts.

Effect of preparation methods on the hydrocracking performance of NiMo/Al_(2)O_(3) catalysts

In this work,NiMo catalysts with various contents of MoO_(3)were prepared through incipient wetness impregnation by a twostep method(NMxA)and onepot method(NMxB).The catalysts were then characterized by XRD,XPS,NH3TPD,H_(2)TPR,HRTEM,and N_(2)adsorptiondesorption technologies.The performance of the NiMo/Al_(2)O_(3) catalysts was investigated by hydrocracking lowtemperature coal tar.When the MoO3 content was 15 wt%,the interaction between Ni species and Al_(2)O_(3) on the NM15B catalyst was stronger than that on the NM15A catalyst,resulting in the poor performance of the former.When the MoO^(3) content was 20 wt%,MoO_(3) agglomerated on the surface of the NM20A catalyst,leading to decreased number of active sites and specific surface area and reduced catalytic performance.The increase in the number of MoS_(2) stack layers strengthened the interaction between Ni and Mo species of the NM20B catalyst and consequently improved its catalytic performance.When the MoO_(3) content reached 25 wt%,the active metals agglomerated on the surface of the NiMo catalysts,thereby directly decreasing the number of active sites.In conclusion,the twostep method is suitable for preparing catalysts with large pore diameter and low MoO_(3) content loading,and the onepot method is more appropriate for preparing catalysts with large specific surface area and high MoO_(3) content.Moreover,the NMxA catalysts had larger average pore diameter than the NMxB catalysts and exhibited improved desulfurization performance.

Effect of preparation methods on Pt/alumina catalysts for the hydrogen iodide catalytic decomposition

Three kinds of Pt/alumina catalysts were prepared by impregnation-hydrogen reduction, impregnation-hydrazine reduction and electroless plating methods. Their differences in the structures, specific areas and particle sizes were characterized by XRD, BET and TEM, respectively. Furthermore, their catalytic activities for the hydrogen iodide （HI） decomposition were evaluated in a fixed bed reactor. The results show that the catalyst 5%Pt/Al2O3 prepared by the electroless plating has the optimum catalytic properties for HI decomposition owing to the high dispersion of the platinum nano-particles （〈5 nm） on the alumina supports.

Comparative Study of Various Preparation Methods of Colloidal Silica

Colloidal silica can be prepared by various methods and starting materials including ion exchange of aqueous silicates, hydrolysis and condensation of silicon compounds, direct oxidation of silicon, and milling and peptization of silica powder. Various silica sols having particle sizes of 10-60 nm prepared by these methods and the preparation methods have been compared on the basis of their shape, size uniformity, sphericity, stability against pH variation, cation concentration, and price, etc. Silica sol prepared from tetraethoxysilane affords uniform size control and growth, and high purity, despite the relatively high costs. Silica sol prepared from liquid silicates affords relatively easy size and shape control;however, it is difficult to lower the alkali content to a level that is appropriate for carrying out semiconductor chemical mechanical polishing processes;in addition, the waste water treatment carried out for recovering the ion exchange resin gives rise environmental consideration. The properties of colloidal silica prepared from fumed silica powder by milling and dispersion depend on the starting silica source and it is relatively difficult to obtain monodispersed particles using this method. Colloidal silica prepared from silicon by direct oxidation has a monodispersed spherical shape and purity control with reasonable prices. It generates less waste water because it can be directly produced in relatively high concentrations. The cation fraction located in the particle relative to the free cation in the fluid is relatively lower in the silica sol prepared by the direct oxidation than others. A careful comparison of colloidal silica and the preparation methods may help in choosing the proper colloidal silica that is the most appropriate for the application being considered.

Classification of Preparation Methods and Wearability of Smart Textiles

In recent years,smart textiles have attracted the attention of scholars from all walks of life,but there is an imbalance between functionality and usability,which affects their marketization process.Firstly,five representative smart textiles are introduced and their respective wearability is described around preparation methods.Secondly,it is concluded that the preparation methods of smart textiles can be divided into two categories:fiber methods and finishing methods.The fiber methods refer to making smart fibers into smart textiles.Textiles made by fiber methods are breathable and feel good in the hand,but the mechanical properties are influenced by the production equipment,and the process cost is high.The finishing methods refer to the functional finishing of ordinary textiles.Although the finishing method is simple and convenient,it may reduce the comfort of the textile.Finally,applications and new research in various fields of smart textiles are presented with promising prospects.It is anticipated that this review will serve as a theoretical basis for future research and development of smart textiles.Researchers are expected to create new technologies to overcome the tension between functionality and usability,as well as to increase user comfort and convenience.

Multifunctional graphene‐based composite photocatalysts oriented by multifaced roles of graphene in photocatalysis

Graphene(GR),a single‐layer carbon sheet with a hexagonal packed lattice structure,has displayed attractive potential and demonstrably become the research focus in artificial photocatalysis due to its enchanting properties in enhancing light absorption,electron transfer dynamics,and surface reactions.Currently,numerous efforts have shown that the properties of GR,which are closely correlated to the photocatalytic performance of GR‐based composites are significantly affected by the synthesis methods.Herein,we first introduce the optimization strategies of GR‐based hybrids and then elaborate the synthesis of GR‐based composite photocatalysts oriented by manifold roles of GR in photoredox catalysis,containing photoelectron mediator and acceptor,improving adsorption capacity,regulating light absorption range and intensity,as well as macromolecular photosensitizer.Beyond that,a brief outlook on the challenges in this burgeoning research field and potential evolution strategies for enhancing the photoactivity of GR‐based hybrids is presented and we anticipate that this review could provide some enlightenments for the rational construction and application of multifunctional GR‐based composite photocatalysts.

Torsional postbuckling characteristics of functionally graded graphene enhanced laminated truncated conical shell with temperature dependent material properties

Buckling and postbuckling characteristics of laminated graphene-enhanced composite(GEC)truncated conical shells exposed to torsion under temperature conditions using finite element method(FEM)simulation are presented in this study.In the thickness direction,the GEC layers of the conical shell are ordered in a piece-wise arrangement of functionally graded(FG)distribution,with each layer containing a variable volume fraction for graphene reinforcement.To calculate the properties of temperaturedependent material of GEC layers,the extended Halpin-Tsai micromechanical framework is used.The FEM model is verified via comparing the current results obtained with the theoretical estimates for homogeneous,laminated cylindrical,and conical shells,the FEM model is validated.The computational results show that a piece-wise FG graphene volume fraction distribution can improve the torque of critical buckling and torsional postbuckling strength.Also,the geometric parameters have a critical impact on the stability of the conical shell.However,a temperature rise can reduce the crucial torsional buckling torque as well as the GEC laminated truncated conical shell’s postbuckling strength.

Structure and synthesis of graphene oxide

Graphene oxide(GO)is one typical two-dimension structured and oxygenated planar molecular material.Researchers across multiple disciplines have paid enormous attention to it due to the unique physiochemical properties.However,models used to describe the structure of GO are still in dispute and ongoing to update.And currently,synthesis methods for mass production are seemingly abundant but in fact,dominated by a few core methodologies.To update with the state-of-art opinions and progresses,herein we present a mini critical review regarding the synthesis of GO as well as its models and simulations of structure.Also,we discuss the perspectives.

Graphene oxide assisted facile hydrothermal synthesis of LiMn_(0.6)Fe_(0.4)PO_4 nanoparticles as cathode material for lithium ion battery

Assisted by graphene oxide（GO）,nano-sized LiMn0.6Fe0.4PO4 with excellent electrochemical performance was prepared by a facile hydrothermal method as cathode material for lithium ion battery.SEM and TEM images indicate that the particle size of LiMn0.6Fe0.4PO4（S2）was about 80 nm in diameter.The discharge capacity of LiMn0.6Fe0.4PO4 nanoparticles was 140.3 mAh-g^1 in the first cycle.It showed that graphene oxide was able to restrict the growth of LiMn0.6Fe0.4PO4 and it in situ reduction of GO could improve the electrical conductivity of LiMn0.6Fe0.4PO4 material.

Simulation on effect of metal/graphene hybrid transparent electrode on characteristics of GaN light emitting diodes

In order to decrease the Schottky barrier height and sheet resistance between graphene （Gr） and the p-GaN layers in GaN-based light-emitting diodes （LEDs）, some transparent thin films with good conductivity and large work function are essential to insert into Gr and p-GaN layers. In this work, the ultra-thin films of four metals （silver （Ag）, golden （Au）, nickel （Ni）, platinum （Pt）） are explored to introduce as a bridge layer into Gr and p-GaN, respectively. The effect of a different combination of Gr/metal transparent conductive layers （TCLs） on the electrical, optical, and thermal characteristics of LED was investigated by the finite element methods. It is found that both the TCLs transmittance and the surface temperature of the LED chip reduces with the increase of the metal thickness, and the transmittance decreases to about 80% with the metal thickness increasing to 2 nm. The surface temperature distribution, operation voltage, and optical output power of the LED chips with different metal/Gr combination were calculated and analyzed. Based on the electrical, optical, and thermal performance of LEDs, it is found that 1.5-nm Ag or Ni or Pt, but 1-nm Au combined with 3 layered （L） Gr is the optimal Gr/metal hybrid transparent and current spreading electrode for ultra-violet （UV） or near-UV LEDs.

Preparing three-dimensional graphene architectures: Review of recent developments

The recent development of synthesis processes to assemble graphene sheets into porous three-dimensional （3D）macroscopic structures are reviewed, including our efforts on 3D graphene structures. Mechanisms for building 3D graphene architectures and their composite materials are also summarized. The functional systems based on 3D graphene architectures provide a significant enhancement in the efficacy due to their unique structures and properties.