Graphene prepared by non-covalent modification of sulfonated poly(ether-ether-ketone)(SPG)was combined with polyvinylidene fluoride(PVDF)/Al to improve the PVDF/Al thermal conductivity while reducing the effect of the...Graphene prepared by non-covalent modification of sulfonated poly(ether-ether-ketone)(SPG)was combined with polyvinylidene fluoride(PVDF)/Al to improve the PVDF/Al thermal conductivity while reducing the effect of the thermal resistance at the graphene-polymer interface.The regulation rule of SPG with different contents on the energy release of fluorine-containing system was studied.When the content of SPG is 4%,the peak pressure and rise rate of SPG/PVDF/Al composite powder during ignition reach the maximum of 4845.28 kPa and 8683.58 kPa/s.When the content of SPG is 5%,the PVDF/Al composite powder is completely coated by SPG,and the calorific value of the material reachs the maximum of 29.094 kJ/g.Through the design and micro-control of the composite powder,the calorific value of the material can be effectively improved,but the improvement of the mass release rate still depends on the graphene content and surface modification state.展开更多
We research the adsorption geometries graphene （Li-GR） before and after CO and electronic structures of pristine graphene （p-GR） and Li-doped adsorption by first-principles. The adsorption energies Ead of CO on p-...We research the adsorption geometries graphene （Li-GR） before and after CO and electronic structures of pristine graphene （p-GR） and Li-doped adsorption by first-principles. The adsorption energies Ead of CO on p-GR and Li-GR are calculated. The results demonstrate that Ead of CO on Li-GR is from -3.3 eV to -3.5 eV, meanwhile Q is up to 0.13e, which indicate that strong electrostatic attractions occur between CO and Li-GR, while CO is physically adsorbed on p-GR. The obvious accumulated charge in electron density difference and increasing carrier density suggest that the conductivity of Li-GR is improved considerably after CO adsorp- tion. An adsorption mechanism is also proposed. Our results provide a path to achieving CO sensors with high performance.展开更多
Few-layer graphenes were fabricated from expandable graphite by rapid microwave exfoliation. Expandable graphite was irradiated in a domestic microwave in full power for 3 min, then soaked in mixed strong hydrogen nit...Few-layer graphenes were fabricated from expandable graphite by rapid microwave exfoliation. Expandable graphite was irradiated in a domestic microwave in full power for 3 min, then soaked in mixed strong hydrogen nitrate and sulfuric acid with volume ratio of 1：1 for 24 h and re-irradiated, thus few-layer graphene sheets were obtained. Specimens gained from every step were selectively characterized by different techniques, such as SEM, XRD, Raman, AFM, XPS, FTIR and combustion elemental analysis. The results show that expandable graphite with loose, porous and worm-like morphology forms instantaneously in microwave irradiation with crackling sound and sparkles, which manifests physical exfoliation of graphene sheets. Few-layer graphene sheets with a dozen or more layers and average thickness of about 4.7 nm are obtained eventually after sequential treatment of microwave irradiation, mixed acid soaking and second microwave irradiation. The as-prepared few-layer graphenes still have high crystallinity and high purity with traces of oxide groups and without serious unrecoverable oxidation damage.展开更多
Adsorption and desorption of hydrogen on/from single-vacancy and double-vacancy graphenes were studied by means of first-principles calculations. The structure and stability of continuous hydrogenation in single vacan...Adsorption and desorption of hydrogen on/from single-vacancy and double-vacancy graphenes were studied by means of first-principles calculations. The structure and stability of continuous hydrogenation in single vacancy were investigated. Several new stable structures were found, along with their corresponding energy barriers. In double-vacancy graphene, the preferred sites of H atoms were identified, and H2 molecule desorption and adsorption of from/on were calculated from the energy barriers. This work provides a systematic and comprehensive understanding of hydrogen behavior on defected graphene.展开更多
In this work we report that when ferromagnetic metals （Fe, Co and Ni） are thermMly evaporated onto n-layer graphenes and graphite, a metal nanowire and adjacent nanogaps can be found along the edges regardless of it...In this work we report that when ferromagnetic metals （Fe, Co and Ni） are thermMly evaporated onto n-layer graphenes and graphite, a metal nanowire and adjacent nanogaps can be found along the edges regardless of its zigzag or armchair structure. Similar features can also be observed for paramagnetic metals, such as Mn, Al and Pd. Meanwhile, metal nanowires and adjacent nanogaps cannot be found for diamagnetic metals （Au and Ag）. An external magnetic field during the evaporation of metals can make these unique features disappear for ferromagnetic and paramagnetic metal; and the morphologies of diamagnetic metal do not change after the application of an external magnetic field. We discuss the possible reasons for these novel and interesting results, which include possible one-dimensional ferromagnets along the edge and edge-related binding energy.展开更多
Friction plays a critical role in the function and maintenance of small-scale structures, where the conventional Coulomb friction law often fails. To probe the friction at small scales, here we present a molecular dyn...Friction plays a critical role in the function and maintenance of small-scale structures, where the conventional Coulomb friction law often fails. To probe the friction at small scales, here we present a molecular dynamics study on the process of dragging graphene nanoribbons on waved graphene substrates. The simulation shows that the induced friction on graphene with zero waviness is ultra-low and closely related to the surface energy barrier. On waved graphenes, the friction generally increases with the amplitude of the wave at a fixed period, but anomalously increases and then decreases with the period at a fixed amplitude. These findings provide the insights into the ultraqow friction at small scales, as well as some guidelines into the fabrication ofgraphene-based nano-composites with high performance.展开更多
The adsorption of hydrogen molecules on titanium-decorated （Ti-decorated） single-layer and bilayer graphenes is studied using density functional theory （DFT） with the relativistic effect. Both the local density ap...The adsorption of hydrogen molecules on titanium-decorated （Ti-decorated） single-layer and bilayer graphenes is studied using density functional theory （DFT） with the relativistic effect. Both the local density approximation （LDA） and the generalized gradient approximation （GGA） are used for obtaining the region of the adsorption energy of H2 molecules on Ti-decorated graphene. We find that a graphene layer with titanium （Ti） atoms adsorbed on both sides can store hydrogen up to 9.51 wt% with average adsorption energy in a range from -0.170 eV to 0.518 eV. Based on the adsorption energy criterion, we find that chemisorption is predominant for H2 molecules when the concentration of H2 molecules absorbed is low while physisorption is predominant when the concentration is high. The computation results for the bilayer graphene decorated with Ti atoms show that the lower carbon layer makes no contribution to hydrogen adsorption.展开更多
In this paper, the epitaxial graphene layers grown on Si- and C-face 6H-SiC substrates are investigated under a low pressure of 400 Pa at 1600℃ By using atomic force microscopy and Raman spectroscopy, we find that th...In this paper, the epitaxial graphene layers grown on Si- and C-face 6H-SiC substrates are investigated under a low pressure of 400 Pa at 1600℃ By using atomic force microscopy and Raman spectroscopy, we find that there are distinct differences in the formation and the properties between the epitaxial graphene layers grown on the Si-face and the C-face substrates, including the hydrogen etching process, the stacking type, and the number of layers. Hopefully, our results will be useful for improving the quality of the epitaxial graphene on SiC substrate.展开更多
A highly efficient catalyst of graphene-supported mixed-valent Mn_(16)-containing polyoxometalate is reported here by electrochemical strategy. The modified electrode with the catalyst exhibits an excellent electrocat...A highly efficient catalyst of graphene-supported mixed-valent Mn_(16)-containing polyoxometalate is reported here by electrochemical strategy. The modified electrode with the catalyst exhibits an excellent electrocatalytic performance for water oxidation, which will contribute to the development of highly efficient catalysts for oxygen evolution.展开更多
The existence of nanographene in cluster form is discussed in organic solvents. Theories are developed based on the columnlet, bundlet and droplet models describing the size-distribution functions. Phenomena present a...The existence of nanographene in cluster form is discussed in organic solvents. Theories are developed based on the columnlet, bundlet and droplet models describing the size-distribution functions. Phenomena present a unified explanation in the columnlet model in which free energy of Cgraphene involved in cluster is combined from a volume part proportional to the number of molecules n in cluster and a constant. The columnlet model enables describing distribution function of Cgraphene clusters by size. From purely geometrical considerations the columnlet （Cgraphene）, bundlet （single-wall carbon nanotube）, CNT （carbon nanotube）, SWNT （single-wall C-nanotube）, and carbon nanobud, CNB （carbon nanobud）） and droplet （fullerene） models predict dissimilar behaviours. The interaction-energy parameters of Cgraphene are taken from C60. An CNB behaviour or further is expected. The decay of solubility with rising temperature is smaller for Cgraphene than for SWNT and CNB and, furthermore, than for C60, in agreement with lesser numbers of units in Cgraphene clusters. The discrepancy between the experimental data of the heat of solution of fullerenes, CNTs, CNBs and graphenes is ascribed to the sharp concentration dependence of the heat of solution. The diffusion coefficient drops with temperature result greater for Cgraphene than CNB and SWNT than C60 corresponding to lesser number of units in clusters. The aggregates near （C60）13, SWNT/CNB7 and （Cgraphene）3 could be representative of the droplet, bundlet and columnlet models.展开更多
In this paper,the epitaxial graphene layers grown on Si-and C-face 6H-SiC substrates are investigated under a low pressure of 400 Pa at 1600 C.By using atomic force microscopy and Raman spectroscopy,we find that there...In this paper,the epitaxial graphene layers grown on Si-and C-face 6H-SiC substrates are investigated under a low pressure of 400 Pa at 1600 C.By using atomic force microscopy and Raman spectroscopy,we find that there are distinct differences in the formation and the properties between the epitaxial graphene layers grown on the Si-face and the C-face substrates,including the hydrogen etching process,the stacking type,and the number of layers.Hopefully,our results will be useful for improving the quality of the epitaxial graphene on SiC substrate.展开更多
In this study,we comprehensively investigated the scaling law for elastic properties of three-dimensional honeycomb-like graphenes(3D graphenes)using hybrid neural network potential-based molecular dynamics simulation...In this study,we comprehensively investigated the scaling law for elastic properties of three-dimensional honeycomb-like graphenes(3D graphenes)using hybrid neural network potential-based molecular dynamics simulations and theoretical analyses.The elastic constants were obtained as functions of honeycomb hole size,denoted by the graphene wall length L.All five independent elastic constants in the large-L limit are proportional to L^(-1).The associated coefficients are combinations of elastic constants of two-dimensional graphene.High-order terms including L^(-2)and L^(-3)emerge for finite L values.They have three origins,the distorted areas close to the joint lines of 3D graphenes,the variation in solid angles between graphene plates,and the bending distortion of graphene plates.Significantly,the chirality becomes essential with decreasing L because the joint line structures are different between the armchair and zigzag-type 3D graphenes.Our findings provide insights into the elastic properties of graphene-based superstructures and can be used for further studies on graphene-based materials.展开更多
Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
Graphene-based thermally conductive composites have been proposed as effective thermal management materials for cooling high-power electronic devices.However,when flexible graphene nanosheets are assembled into macros...Graphene-based thermally conductive composites have been proposed as effective thermal management materials for cooling high-power electronic devices.However,when flexible graphene nanosheets are assembled into macroscopic thermally conductive composites,capillary forces induce shrinkage of graphene nanosheets to form wrinkles during solution-based spontaneous drying,which greatly reduces the thermal conductivity of the composites.Herein,graphene nanosheets/aramid nanofiber(GNS/ANF)composite films with high thermal conductivity were prepared by in-plane stretching of GNS/ANF composite hydrogel networks with hydrogen bonds andπ-πinteractions.The in-plane mechanical stretching eliminates graphene nanosheets wrinkles by suppressing inward shrinkage due to capillary forces during drying and achieves a high in-plane orientation of graphene nanosheets,thereby creating a fast in-plane heat transfer channel.The composite films(GNS/ANF-60 wt%)with eliminated graphene nanosheets wrinkles showed a significant increase in thermal conductivity(146 W m^(−1)K^(−1))and tensile strength(207 MPa).The combination of these excellent properties enables the GNS/ANF composite films to be effectively used for cooling flexible LED chips and smartphones,showing promising applications in the thermal management of high-power electronic devices.展开更多
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...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.展开更多
Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herei...Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herein,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite networks.The mechanism of biological adsorption assembly is also proposed.As a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes.In this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized.Meanwhile,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides.Accordingly,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.展开更多
Recently,the increasing interest in wearable technology for personal healthcare and smart virtual/augmented reality applications has led to the development of facile fabrication methods.Lasers have long been used to d...Recently,the increasing interest in wearable technology for personal healthcare and smart virtual/augmented reality applications has led to the development of facile fabrication methods.Lasers have long been used to develop original solutions to such challenging technological problems due to their remote,sterile,rapid,and site-selective processing of materials.In this review,recent developments in relevant laser processes are summarized under two separate categories.First,transformative approaches,such as for laser-induced graphene,are introduced.In addition to design optimization and the alteration of a native substrate,the latest advances under a transformative approach now enable more complex material compositions and multilayer device configurations through the simultaneous transformation of heterogeneous precursors,or the sequential addition of functional layers coupled with other electronic elements.In addition,the more conventional laser techniques,such as ablation,sintering,and synthesis,can still be used to enhance the functionality of an entire system through the expansion of applicable materials and the adoption of new mechanisms.Later,various wearable device components developed through the corresponding laser processes are discussed,with an emphasis on chemical/physical sensors and energy devices.In addition,special attention is given to applications that use multiple laser sources or processes,which lay the foundation for the all-laser fabrication of wearable devices.展开更多
For the porous‐membrane‐based osmotic energy generator,the potential synergistic enhancement mechanism of various key parameters is still controversial,especially because optimizing the trade‐off between permeabili...For the porous‐membrane‐based osmotic energy generator,the potential synergistic enhancement mechanism of various key parameters is still controversial,especially because optimizing the trade‐off between permeability and selectivity is still a challenge.Here,to construct a permeability and selectivity synergistically enhanced osmotic energy generator,the twodimensional porous membranes with tunable charge density are prepared by inserting sulfonated polyether sulfone into graphene oxide.Influences of charge density and pore size on the ion transport are explored,and the ionic behaviors in the channel are calculated by numerical simulations.The mechanism of ion transport in the process is studied in depth,and the fundamental principles of energy conversion are revealed.The results demonstrate that charge density and pore size should be matched to construct the optimal ion channel.This collaborative enhancement strategy of permeability and selectivity has significantly improved the output power in osmotic energy generation;compared to the pure graphene oxide membrane,the composite membrane presents almost 20 times improvement.展开更多
Stemming from the unique in-plane honeycomb lattice structure and the sp^(2)hybridized carbon atoms bonded by exceptionally strong carbon–carbon bonds,graphene exhibits remarkable anisotropic electrical,mechanical,an...Stemming from the unique in-plane honeycomb lattice structure and the sp^(2)hybridized carbon atoms bonded by exceptionally strong carbon–carbon bonds,graphene exhibits remarkable anisotropic electrical,mechanical,and thermal properties.To maximize the utilization of graphene’s in-plane properties,pre-constructed and aligned structures,such as oriented aerogels,films,and fibers,have been designed.The unique combination of aligned structure,high surface area,excellent electrical conductivity,mechanical stability,thermal conductivity,and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions,enabling advancements in diverse fields.This review provides a comprehensive overview of recent advances in highly aligned graphene aerogels and their composites.It highlights the fabrication methods of aligned graphene aerogels and the optimization of alignment which can be estimated both qualitatively and quantitatively.The oriented scaffolds endow graphene aerogels and their composites with anisotropic properties,showing enhanced electrical,mechanical,and thermal properties along the alignment at the sacrifice of the perpendicular direction.This review showcases remarkable properties and applications of aligned graphene aerogels and their composites,such as their suitability for electronics,environmental applications,thermal management,and energy storage.Challenges and potential opportunities are proposed to offer new insights into prospects of this material.展开更多
基金Funded by the National Natural Science Foundation of China(No.52104363)。
文摘Graphene prepared by non-covalent modification of sulfonated poly(ether-ether-ketone)(SPG)was combined with polyvinylidene fluoride(PVDF)/Al to improve the PVDF/Al thermal conductivity while reducing the effect of the thermal resistance at the graphene-polymer interface.The regulation rule of SPG with different contents on the energy release of fluorine-containing system was studied.When the content of SPG is 4%,the peak pressure and rise rate of SPG/PVDF/Al composite powder during ignition reach the maximum of 4845.28 kPa and 8683.58 kPa/s.When the content of SPG is 5%,the PVDF/Al composite powder is completely coated by SPG,and the calorific value of the material reachs the maximum of 29.094 kJ/g.Through the design and micro-control of the composite powder,the calorific value of the material can be effectively improved,but the improvement of the mass release rate still depends on the graphene content and surface modification state.
基金Supported by the National Natural Science Foundation of China under Grant Nos 51372282,51072024 and 51132002the National College Students’Innovative and Entrepreneurial Training Program of Beijing Institute of Technology under Grant No201410007050
文摘We research the adsorption geometries graphene （Li-GR） before and after CO and electronic structures of pristine graphene （p-GR） and Li-doped adsorption by first-principles. The adsorption energies Ead of CO on p-GR and Li-GR are calculated. The results demonstrate that Ead of CO on Li-GR is from -3.3 eV to -3.5 eV, meanwhile Q is up to 0.13e, which indicate that strong electrostatic attractions occur between CO and Li-GR, while CO is physically adsorbed on p-GR. The obvious accumulated charge in electron density difference and increasing carrier density suggest that the conductivity of Li-GR is improved considerably after CO adsorp- tion. An adsorption mechanism is also proposed. Our results provide a path to achieving CO sensors with high performance.
基金Project(51274248)supported by the National Natural Science Foundation of China
文摘Few-layer graphenes were fabricated from expandable graphite by rapid microwave exfoliation. Expandable graphite was irradiated in a domestic microwave in full power for 3 min, then soaked in mixed strong hydrogen nitrate and sulfuric acid with volume ratio of 1：1 for 24 h and re-irradiated, thus few-layer graphene sheets were obtained. Specimens gained from every step were selectively characterized by different techniques, such as SEM, XRD, Raman, AFM, XPS, FTIR and combustion elemental analysis. The results show that expandable graphite with loose, porous and worm-like morphology forms instantaneously in microwave irradiation with crackling sound and sparkles, which manifests physical exfoliation of graphene sheets. Few-layer graphene sheets with a dozen or more layers and average thickness of about 4.7 nm are obtained eventually after sequential treatment of microwave irradiation, mixed acid soaking and second microwave irradiation. The as-prepared few-layer graphenes still have high crystallinity and high purity with traces of oxide groups and without serious unrecoverable oxidation damage.
基金supported by the National Natural Science Foundation of China(Grant No.5160121211475082)‘‘Strategic Priority Research Program of Chinese Academy of Sciences’’ Thorium Molten Salts Reactor Fund
文摘Adsorption and desorption of hydrogen on/from single-vacancy and double-vacancy graphenes were studied by means of first-principles calculations. The structure and stability of continuous hydrogenation in single vacancy were investigated. Several new stable structures were found, along with their corresponding energy barriers. In double-vacancy graphene, the preferred sites of H atoms were identified, and H2 molecule desorption and adsorption of from/on were calculated from the energy barriers. This work provides a systematic and comprehensive understanding of hydrogen behavior on defected graphene.
基金supported by the National Natural Science Foundation of China (Grant Nos. 10774032,90921001 and 50952009)
文摘In this work we report that when ferromagnetic metals （Fe, Co and Ni） are thermMly evaporated onto n-layer graphenes and graphite, a metal nanowire and adjacent nanogaps can be found along the edges regardless of its zigzag or armchair structure. Similar features can also be observed for paramagnetic metals, such as Mn, Al and Pd. Meanwhile, metal nanowires and adjacent nanogaps cannot be found for diamagnetic metals （Au and Ag）. An external magnetic field during the evaporation of metals can make these unique features disappear for ferromagnetic and paramagnetic metal; and the morphologies of diamagnetic metal do not change after the application of an external magnetic field. We discuss the possible reasons for these novel and interesting results, which include possible one-dimensional ferromagnets along the edge and edge-related binding energy.
基金support of the Science and Technology Development Fund from Macao SAR (FDCT-068/2014/A2 and FDCT-132/2014/A3) Multi-Year Research Grants (MYRG201400159-FST and MYRG2015-00017-FST) from Research & Development Office at University of Macaosupport of the National Natural Science Foundation of China (Grant No.11372279)
文摘Friction plays a critical role in the function and maintenance of small-scale structures, where the conventional Coulomb friction law often fails. To probe the friction at small scales, here we present a molecular dynamics study on the process of dragging graphene nanoribbons on waved graphene substrates. The simulation shows that the induced friction on graphene with zero waviness is ultra-low and closely related to the surface energy barrier. On waved graphenes, the friction generally increases with the amplitude of the wave at a fixed period, but anomalously increases and then decreases with the period at a fixed amplitude. These findings provide the insights into the ultraqow friction at small scales, as well as some guidelines into the fabrication ofgraphene-based nano-composites with high performance.
基金supported by the National Natural Science Foundation of China (Grant Nos. 10974076,11047020,and 11204120)the Natural Science Foundation of Shandong Province,China (Grant No. ZR2012AM022)
文摘The adsorption of hydrogen molecules on titanium-decorated （Ti-decorated） single-layer and bilayer graphenes is studied using density functional theory （DFT） with the relativistic effect. Both the local density approximation （LDA） and the generalized gradient approximation （GGA） are used for obtaining the region of the adsorption energy of H2 molecules on Ti-decorated graphene. We find that a graphene layer with titanium （Ti） atoms adsorbed on both sides can store hydrogen up to 9.51 wt% with average adsorption energy in a range from -0.170 eV to 0.518 eV. Based on the adsorption energy criterion, we find that chemisorption is predominant for H2 molecules when the concentration of H2 molecules absorbed is low while physisorption is predominant when the concentration is high. The computation results for the bilayer graphene decorated with Ti atoms show that the lower carbon layer makes no contribution to hydrogen adsorption.
基金Project supported by the Key Research Foundation from the Ministry of Education of China （Grant No. JY10000925016）.
文摘In this paper, the epitaxial graphene layers grown on Si- and C-face 6H-SiC substrates are investigated under a low pressure of 400 Pa at 1600℃ By using atomic force microscopy and Raman spectroscopy, we find that there are distinct differences in the formation and the properties between the epitaxial graphene layers grown on the Si-face and the C-face substrates, including the hydrogen etching process, the stacking type, and the number of layers. Hopefully, our results will be useful for improving the quality of the epitaxial graphene on SiC substrate.
基金supported by the National Natural Science Foundation of China(No.21371173,51402298,91545125)the China Postdoctoral Foundation(No.2014M550846)
文摘A highly efficient catalyst of graphene-supported mixed-valent Mn_(16)-containing polyoxometalate is reported here by electrochemical strategy. The modified electrode with the catalyst exhibits an excellent electrocatalytic performance for water oxidation, which will contribute to the development of highly efficient catalysts for oxygen evolution.
文摘The existence of nanographene in cluster form is discussed in organic solvents. Theories are developed based on the columnlet, bundlet and droplet models describing the size-distribution functions. Phenomena present a unified explanation in the columnlet model in which free energy of Cgraphene involved in cluster is combined from a volume part proportional to the number of molecules n in cluster and a constant. The columnlet model enables describing distribution function of Cgraphene clusters by size. From purely geometrical considerations the columnlet （Cgraphene）, bundlet （single-wall carbon nanotube）, CNT （carbon nanotube）, SWNT （single-wall C-nanotube）, and carbon nanobud, CNB （carbon nanobud）） and droplet （fullerene） models predict dissimilar behaviours. The interaction-energy parameters of Cgraphene are taken from C60. An CNB behaviour or further is expected. The decay of solubility with rising temperature is smaller for Cgraphene than for SWNT and CNB and, furthermore, than for C60, in agreement with lesser numbers of units in Cgraphene clusters. The discrepancy between the experimental data of the heat of solution of fullerenes, CNTs, CNBs and graphenes is ascribed to the sharp concentration dependence of the heat of solution. The diffusion coefficient drops with temperature result greater for Cgraphene than CNB and SWNT than C60 corresponding to lesser number of units in clusters. The aggregates near （C60）13, SWNT/CNB7 and （Cgraphene）3 could be representative of the droplet, bundlet and columnlet models.
基金Project supported by the Key Research Foundation from the Ministry of Education of China (Grant No. JY10000925016)
文摘In this paper,the epitaxial graphene layers grown on Si-and C-face 6H-SiC substrates are investigated under a low pressure of 400 Pa at 1600 C.By using atomic force microscopy and Raman spectroscopy,we find that there are distinct differences in the formation and the properties between the epitaxial graphene layers grown on the Si-face and the C-face substrates,including the hydrogen etching process,the stacking type,and the number of layers.Hopefully,our results will be useful for improving the quality of the epitaxial graphene on SiC substrate.
基金supported by the National Natural Science Foundation of China(Grant Nos.12022415,11974056,and 12074271)。
文摘In this study,we comprehensively investigated the scaling law for elastic properties of three-dimensional honeycomb-like graphenes(3D graphenes)using hybrid neural network potential-based molecular dynamics simulations and theoretical analyses.The elastic constants were obtained as functions of honeycomb hole size,denoted by the graphene wall length L.All five independent elastic constants in the large-L limit are proportional to L^(-1).The associated coefficients are combinations of elastic constants of two-dimensional graphene.High-order terms including L^(-2)and L^(-3)emerge for finite L values.They have three origins,the distorted areas close to the joint lines of 3D graphenes,the variation in solid angles between graphene plates,and the bending distortion of graphene plates.Significantly,the chirality becomes essential with decreasing L because the joint line structures are different between the armchair and zigzag-type 3D graphenes.Our findings provide insights into the elastic properties of graphene-based superstructures and can be used for further studies on graphene-based materials.
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.
基金the National Natural Science Foundation of China(No.51972162).
文摘Graphene-based thermally conductive composites have been proposed as effective thermal management materials for cooling high-power electronic devices.However,when flexible graphene nanosheets are assembled into macroscopic thermally conductive composites,capillary forces induce shrinkage of graphene nanosheets to form wrinkles during solution-based spontaneous drying,which greatly reduces the thermal conductivity of the composites.Herein,graphene nanosheets/aramid nanofiber(GNS/ANF)composite films with high thermal conductivity were prepared by in-plane stretching of GNS/ANF composite hydrogel networks with hydrogen bonds andπ-πinteractions.The in-plane mechanical stretching eliminates graphene nanosheets wrinkles by suppressing inward shrinkage due to capillary forces during drying and achieves a high in-plane orientation of graphene nanosheets,thereby creating a fast in-plane heat transfer channel.The composite films(GNS/ANF-60 wt%)with eliminated graphene nanosheets wrinkles showed a significant increase in thermal conductivity(146 W m^(−1)K^(−1))and tensile strength(207 MPa).The combination of these excellent properties enables the GNS/ANF composite films to be effectively used for cooling flexible LED chips and smartphones,showing promising applications in the thermal management of high-power electronic devices.
基金supported by National Natural Science Foundation of China (NSFC 52372041, 52302087, 51772060, 51672059 and 51621091)Heilongjiang Touyan Team Program+1 种基金the Fundamental Research Funds for the Central Universities (Grant No. HIT.OCEF.2021003)the Shanghai Aerospace Science and Technology Innovation Fund (SAST2022-60)。
文摘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.
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金Natural Science Foundation for Distinguished Young Scholars of Zhejiang Province,Grant/Award Number:LR20E020001Foundation of State Key Laboratory of Coal Conversion,Grant/Award Number:J20-21-909+4 种基金Science and Technology Department of Zhejiang Province,Grant/Award Number:2023C01231National Natural Science Foundation of China,Grant/Award Numbers:52372235,52073252,52002052,22379020,U20A20253,21972127,22279116Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment,Grant/Award Number:SKLPEE-KF202206Key Research and Development Project of Science and Technology Department of Sichuan Province,Grant/Award Number:2022YFSY0004Ministry of Education,Grant/Award Number:KFM 202202。
文摘Ingenious design and fabrication of advanced carbon-based sulfur cathodes are extremely important to the development of high-energy lithium-sulfur batteries,which hold promise as the next-generation power source.Herein,for the first time,we report a novel versatile hyphae-mediated biological assembly technology to achieve scale production of hyphae carbon fibers(HCFs)derivatives,in which different components including carbon,metal compounds,and semiconductors can be homogeneously assembled with HCFs to form composite networks.The mechanism of biological adsorption assembly is also proposed.As a representative,reduced graphene oxides(rGOs)decorated with hollow carbon spheres(HCSs)successfully co-assemble with HCFs to form HCSs@rGOs/HCFs hosts for sulfur cathodes.In this unique architecture,not only large accommodation space for sulfur but also restrained volume expansion and fast charge transport paths are realized.Meanwhile,multiscale physical barriers plus chemisorption sites are simultaneously established to anchor soluble lithium polysulfides.Accordingly,the designed HCSs@rGOs/HCFs-S cathodes deliver a high capacity(1189 mA h g^(-1)at 0.1 C)and good high-rate capability(686 mA h g^(-1)at 5 C).Our work provides a new approach for the preparation of high-performance carbon-based electrodes for energy storage devices.
基金supported by the Basic Research Program through the National Research Foundation of Korea(NRF)(Nos.2022R1C1C1006593,2022R1A4A3031263,and RS-2023-00271166)the National Science Foundation(Nos.2054098 and 2213693)+1 种基金the National Natural Science Foundation of China(No.52105593)Zhejiang Provincial Natural Science Foundation of China(No.LDQ24E050001).EH acknowledges a fellowship from the Hyundai Motor Chung Mong-Koo Foundation.
文摘Recently,the increasing interest in wearable technology for personal healthcare and smart virtual/augmented reality applications has led to the development of facile fabrication methods.Lasers have long been used to develop original solutions to such challenging technological problems due to their remote,sterile,rapid,and site-selective processing of materials.In this review,recent developments in relevant laser processes are summarized under two separate categories.First,transformative approaches,such as for laser-induced graphene,are introduced.In addition to design optimization and the alteration of a native substrate,the latest advances under a transformative approach now enable more complex material compositions and multilayer device configurations through the simultaneous transformation of heterogeneous precursors,or the sequential addition of functional layers coupled with other electronic elements.In addition,the more conventional laser techniques,such as ablation,sintering,and synthesis,can still be used to enhance the functionality of an entire system through the expansion of applicable materials and the adoption of new mechanisms.Later,various wearable device components developed through the corresponding laser processes are discussed,with an emphasis on chemical/physical sensors and energy devices.In addition,special attention is given to applications that use multiple laser sources or processes,which lay the foundation for the all-laser fabrication of wearable devices.
基金Natural Science Foundation of Jilin Province,Grant/Award Number:YDZJ202101ZYTS002National Natural Science Foundation of China,Grant/Award Number:52003099+1 种基金Capital Construction Fund of Jilin Province,Grant/Award Number:2021C039‐1Fundamental Research Funds for the Central Universities。
文摘For the porous‐membrane‐based osmotic energy generator,the potential synergistic enhancement mechanism of various key parameters is still controversial,especially because optimizing the trade‐off between permeability and selectivity is still a challenge.Here,to construct a permeability and selectivity synergistically enhanced osmotic energy generator,the twodimensional porous membranes with tunable charge density are prepared by inserting sulfonated polyether sulfone into graphene oxide.Influences of charge density and pore size on the ion transport are explored,and the ionic behaviors in the channel are calculated by numerical simulations.The mechanism of ion transport in the process is studied in depth,and the fundamental principles of energy conversion are revealed.The results demonstrate that charge density and pore size should be matched to construct the optimal ion channel.This collaborative enhancement strategy of permeability and selectivity has significantly improved the output power in osmotic energy generation;compared to the pure graphene oxide membrane,the composite membrane presents almost 20 times improvement.
基金The financial support by the National Natural Science Foundation of China(No.52002020)is acknowledged.
文摘Stemming from the unique in-plane honeycomb lattice structure and the sp^(2)hybridized carbon atoms bonded by exceptionally strong carbon–carbon bonds,graphene exhibits remarkable anisotropic electrical,mechanical,and thermal properties.To maximize the utilization of graphene’s in-plane properties,pre-constructed and aligned structures,such as oriented aerogels,films,and fibers,have been designed.The unique combination of aligned structure,high surface area,excellent electrical conductivity,mechanical stability,thermal conductivity,and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions,enabling advancements in diverse fields.This review provides a comprehensive overview of recent advances in highly aligned graphene aerogels and their composites.It highlights the fabrication methods of aligned graphene aerogels and the optimization of alignment which can be estimated both qualitatively and quantitatively.The oriented scaffolds endow graphene aerogels and their composites with anisotropic properties,showing enhanced electrical,mechanical,and thermal properties along the alignment at the sacrifice of the perpendicular direction.This review showcases remarkable properties and applications of aligned graphene aerogels and their composites,such as their suitability for electronics,environmental applications,thermal management,and energy storage.Challenges and potential opportunities are proposed to offer new insights into prospects of this material.
