In this study,the holey graphene was prepared by microwave-assisted chemical etching.The three-dimensional(3D)holey graphene hydrogel was obtained through hydrothermal self-assembly method,followed by the introduction...In this study,the holey graphene was prepared by microwave-assisted chemical etching.The three-dimensional(3D)holey graphene hydrogel was obtained through hydrothermal self-assembly method,followed by the introduction of FeCo_(2)S_(4)particles.The resulting holey graphene hydrogel,characterized by high specific surface area and abundant pores combined with FeCo_(2)S_(4)with high pseudocapacitance by interfacial interaction,shortened the mass transport path and enhanced the specific capacitance.The findings reveal that the holey graphene hydrogel/FeCo_(2)S_(4)(FeCo_(2)S_(4)/HGH)composite exhibits high specific capacitance and impressive rate capability(413.4 F·g^(-1)at 1 A·g^(-1),300.4 F·g^(-1)at 6 A·g^(-1)).The symmetric supercapacitor operated within a stable potential window of 0.1-1.6 V,achieving specific capacitance of 127.5 F·g^(-1)at 1 A·g^(-1),and can deliver 37.1 Wh·kg^(-1)at a power density of 1499 W·kg^(-1).Besides,under the current density of 3 A·g^(-1),the supercapacitor retained 90.8%of its capacitance after 5000 cycles,demonstrating exceptional cycle stability.This study presents an efficient method for fabricating advanced integrated supercapacitors electrodes with enhanced energy density.展开更多
An efficient chamber-induced activation method was applied for the preparation of holey graphene/cellulose nanofiber-based film with high specific surface area(SSA)and multiple channels through the graphene nanosheets...An efficient chamber-induced activation method was applied for the preparation of holey graphene/cellulose nanofiber-based film with high specific surface area(SSA)and multiple channels through the graphene nanosheets.With the cellulose nanofiber(CNF)simultaneously serving as“dispersing agent,”“spacer,”and“activating agent,”the graphene oxide(GO)nanosheets are perforated by the pyrolysis gas from CNF in the confined space inside the hybrid films,uniformly dispersed,and sandwiched between CNF networks with less agglomeration and restacking.Additionally,we have proved that H2O and H2 are primarily responsible for the activation and etching of GO/CNF film.As the CNF content increases,the mesoporosity of the activated reduced GO/CNF(A-RGO/CNF)film increases,and the graphene nanosheets show more nanopore perforations.Benefitting from the high SSA,high density,moderate mesoporosity,and abundant channels for ion diffusion through the graphene nanosheets,the A-RGO/CNF film exhibits the highest specific capacitance of 323(236)F g^(−1)(F cm^(−3))at 1Ag^(−1).For the A-RGO5/CNF5 film containing half CNF and half GO,an excellent comprehensive electrochemical performance including superior rate performance(208(160)F g^(−1)(F cm^(−3))at 60Ag^(−1))is exhibited.Moreover,the A-RGO5/CNF5 electrode in an all-solid-state flexible symmetric supercapacitor delivers a high specific capacitance of 250(193)F g^(−1)(F cm^(−3))at 1Ag^(−1).This study provides a novel idea for the preparation of holey graphene-based film for supercapacitor electrodes.The strategy of simultaneously employing CNF as“dispersing agent,”“spacer,”and“activating agent”also offers a new vision for the assembly of homogeneous nanohybrid material and the utilization of pyrolysis gas.展开更多
The oxygen evolution reaction(OER)is a half-reaction of water electrolysis,and the OER performance of an electrocatalyst is significantly related to its energy conversion efficiency.Due to their high OER activity,tran...The oxygen evolution reaction(OER)is a half-reaction of water electrolysis,and the OER performance of an electrocatalyst is significantly related to its energy conversion efficiency.Due to their high OER activity,transition metal-based nanomaterials have become potential low-cost substitutes for Ir/Ru-based OER electrocatalysts in an alkaline environment.Herein,holey Fe3O4-coupled Ni(OH)2 sheets(Ni(OH)2-Fe H-STs)were easily achieved by a simple mixed-cyanogel hydrolysis strategy.The two-dimensional(2D)Ni(OH)2-Fe H-STs with ca.1 nm thickness have a high specific surface area,abundant unsaturated coordination atoms,and numerous pores,which are highly favorable for electrocatalytic reactions.Meanwhile,the introduction of Fe improves the conductivity and regulates the electronic structure of Ni.Due to their special structural features and synergistic effect between the Fe and Ni atoms,Ni(OH)2-Fe H-STs with an optimal Ni/Fe ratio show excellent OER activity in a 1 M KOH solution,which significantly exceeds that of the commercial RuO2 nanoparticle electrocatalyst.Furthermore,Ni(OH)2-Fe H-STs can be grown on nickel foam(NF),and the resulting material exhibits enhanced OER activity,such as a small overpotential of 200 mV and a small Tafel slope of 56 mV dec−1,than that of Ni(OH)2-Fe H-STs without NF.展开更多
MXene has given great promises to superca-pacitor electrode material due to its high conductivity and redox properties.However,the self-agglomeration of the MXene lamella will reduce its contact area with the elec-tro...MXene has given great promises to superca-pacitor electrode material due to its high conductivity and redox properties.However,the self-agglomeration of the MXene lamella will reduce its contact area with the elec-trolyte and generate a tortuous transportation pathway of the electrolyte ions,thereby reducing its capacitive per-formance and rate capability.In this work,we engineered the electrolyte ion channels by adjusting the MXene lamella size and inserting holey graphene(HG)nanosheets into the interlayer of the MXene flakes.The developed MXene/HG electrode can not only avoid the self-restack-ing of MXene but also provide unimpeded ion transport channels.As a result,the supercapacitive and rate perfor-mances of the small MXene lamella-based MXene/HG(S-MXene/HG)supercapacitor are prominently ameliorated.By adjusting the content of HG,the S-MXene/HG0.05 electrode exhibits excellent gravimetric capacitance of 446 F·g^(-1)and a rate capability of 77.5%.The S-MXene/HG0.05-based symmetric supercapacitor provides an impressive energy density of 14.84 Wh·kg^(-1)with excellent cyclic stability of 96%capacitance retention after 10,000 cycles.This demonstration of the engineering of the ion channels shows great potential in two-dimensional mate-rial-based supercapacitor electrodes.展开更多
Three-dimensional holey nitrogen-doped carbon matrixes decorated with molybdenum dioxide(MoO_(2))nanoparticles have been successfully synthesized via a NaCl-assisted template strategy.The obtained MoO_(2)/C composites...Three-dimensional holey nitrogen-doped carbon matrixes decorated with molybdenum dioxide(MoO_(2))nanoparticles have been successfully synthesized via a NaCl-assisted template strategy.The obtained MoO_(2)/C composites offered multi-advantages,including higher specific surface area,more active sites,more ions/electrons transmission channels,and shorter transmission path due to the synergistic effect of the uniformly distributed MoO_(2) nanoparticles and porous carbon structure.Especially,the oxygen vacancies were introduced into the prepared composites and enhanced the Li^(+)intercalation/deintercalation process during electrochemical cycling by the Coulomb force.The existence of the local built-in electric field was proved by experimental data,differential charge density distribution,and density of states calculation.The uniquely designed structure and introduced oxygen vacancy defects endowed the MoO_(2)/C composites with excellent electrochemical properties.In view of the synergistic effect of the uniquely designed morphology and introduced oxygen vacancy defects,the MoO_(2)/C composites exhibited superior electrochemical performance of a high capacity of 918.2 mAh g^(-1) at 0.1 A g^(-1) after 130 cycles,562.1 mAh g^(-1) at 1.0 A g^(-1) after 1000 cycles,and a capacity of 181.25 mAh g^(-1) even at 20.0 A g^(-1).This strategy highlights the path to promote the commercial application of MoO_(2)-based and other transition metal oxide electrodes for energy storage devices.展开更多
Porous structure and heteroatom doping are two key parameters for significantly boosting the capacitive performance of graphene-based materials.Herein,we report a facile approach to prepare onedimensional(ID) nitrogen...Porous structure and heteroatom doping are two key parameters for significantly boosting the capacitive performance of graphene-based materials.Herein,we report a facile approach to prepare onedimensional(ID) nitrogen-doped holey graphene nanoscrolls(NHGNSs) through cold quenching treatment of two-dimensional graphene oxide sheets,followed by thermal annealing in the successive atmosphere of NH3 and air.Benefiting from the synergy of the unique 1D tubular morphology,abundant nanoholes and nitrogen doping,the NHGNSs exhibit a high specific capacitance of 126 F/g at 1 A/g in ionic liquid electrolyte and excellent rate capability with 81% of the capacitance retained at 20 A/g.Furthermore,the fabricated symmetric supercapacitors based on NHGNSs achieve both high energy density of 53.5 Wh/kg at 875 W/kg and high power density of 17.5 kW/kg at 43.4 Wh/kg.The simple synthetic process and superior electrochemical performance suggest the great potential of NHGNSs for supercapacitor application.展开更多
Lithium ion batteries(LIBs)have been widely used in portable and smart devices because of their high energy densities,long cycle life and environmental friendliness.In order to meet the evergrowing demand for human-be...Lithium ion batteries(LIBs)have been widely used in portable and smart devices because of their high energy densities,long cycle life and environmental friendliness.In order to meet the evergrowing demand for human-beings utilizing electronic devices,electric vehicles and energy storage grids.展开更多
Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to syn...Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to synthesize the high-quality holey platinum nanotubes(Pt-H-NTs)using nanorods-like Pt^(Ⅱ)-phenanthroline(PT)coordination compound as self-template and self-reduction precursor.Then,an up-bottom strategy is used to further synthesize polyallylamine(PA)modified Pt-H-NTs(Pt-HNTs@PA).PA modification sharply promotes the catalytic activity of Pt-H-NTs for the formic acid electrooxidation reaction(FAEOR)by the direct reaction pathway.Meanwhile,PA modification also elevates the catalytic activity of Pt-H-NTs for the hydrogen evolution reaction(HER)by the proton enrichment at electrolyte/electrode interface.Benefiting from the high catalytic activity of Pt-H-NTs@PA for both FAEOR and HER,a two-electrode FAEOR boosted water electrolysis system is fabricated by using Pt-H-NTs@PA as bifunctio nal electrocatalysts.Such FAEOR boosted water electrolysis system only requires the operational voltage of 0.47 V to achieve the high-purity hydrogen production,showing an energy-saving hydrogen production strategy compared to traditional water electrolysis system.展开更多
In order to design birefringent holey fiber with beat-length independent of wavelength, an asymmetric structure is introduced to reduce its wavelength-sensitivity. The influence of structural parameters on the modal b...In order to design birefringent holey fiber with beat-length independent of wavelength, an asymmetric structure is introduced to reduce its wavelength-sensitivity. The influence of structural parameters on the modal birefringence is calculated and analyzed. After optimizing the parameters, a flat dispersion curve of beat-length is obtained. The beat-length changes from 89.8 mm to 91.0 mm in wavelength range from 1.1 μm, to 1.7μm, and its relative variation is 1.38%. If this fiber is made into zero-order quarter wave plate, the phase delay can be easily controlled in （90±1）°.展开更多
The high power holey fiber is an efficient supercontinuum light source by using picosecond pulse,which is a less expensive laser source compared with low power and expensive femtosecond laser sources. In this paper, a...The high power holey fiber is an efficient supercontinuum light source by using picosecond pulse,which is a less expensive laser source compared with low power and expensive femtosecond laser sources. In this paper, a high power highly nonlinear holey fiber(HN-HF) with a low confinement loss is proposed for supercontinuum light sources. The finite difference method is used to calculate the different properties of the proposed HN-HF. High nonlinear coefficients are obtained at 1.06 μm, 1.31μm, and 1.55μm wavelengths with flattened chromatic dispersion and low confinement losses simultaneously. Moreover, numerical simulation results show that high power broad supercontinuum spectra with very short length of the proposed photonic crystal fiber are achieved.展开更多
This paper proposes three kinds of tapered holey fibres with a multi-layer of holes whose pitch of air holes at the end of untapered and tapered are 5.8 μm and 1.8 μm. The central wavelength which locates in the ano...This paper proposes three kinds of tapered holey fibres with a multi-layer of holes whose pitch of air holes at the end of untapered and tapered are 5.8 μm and 1.8 μm. The central wavelength which locates in the anomalous dispersion region is 1.55 μm. An adaptive split-step Fourier method is numerically used to study the pulse propagation in tapered holey fibres. For the considered convex tapered holey fibre, at a wavelength of 1.55 μm, a compression factor of 136.7 can be achieved by initial width of 800 fs propagation through a length of 0.8 m. It demonstrates that in anomalous dispersion region, pulse can be compressed with the increase of nonlinearity coefficient and the decrease of dispersion coefficient.展开更多
In this study,we introduce and experimentally validate,to our knowledge,a new type of terahertz(THz)fiber waveguide.The waveguide features a core made from petroleum jelly(commonly known as Vaseline)and a cladding mad...In this study,we introduce and experimentally validate,to our knowledge,a new type of terahertz(THz)fiber waveguide.The waveguide features a core made from petroleum jelly(commonly known as Vaseline)and a cladding made of holey polytetrafluoroethylene(PTFE),also known as Teflon.Since the core is biocompatible and the cladding is safe for human use,this design has promising applications for biocompatible probes in the THz range.We rigorously analyzed the transmission properties of the waveguide using the finite element method(FEM)and followed up with experimental validation using a THz time-domain spectroscopy(THz-TDS)system.The fiber supports single-mode operation for frequencies below 0.9 THz and demonstrates low-loss transmission of THz waves,even when tightly bent.For instance,with a bending radius as small as 1.61 cm,the fiber exhibited minimal losses of 0.23 dB/cm at 0.2 THz and 0.27 dB/cm at 0.5 THz,surpassing previous technical limitations.Another key advantage is the strong confinement of the THz waves within the petroleum jelly core,which helps maintain low dispersion and ensures stable pulse transmission,even under tight bends.The exceptional stability and flexibility of this biocompatible THz fiber make it highly suitable for sensing and imaging applications in confined,flexible environments,including potential uses within the human body.展开更多
A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes,involving direci eating of mixtures of melamine and urea or melamine and cyanuric acid in specifi...A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes,involving direci eating of mixtures of melamine and urea or melamine and cyanuric acid in specific mass ratios.Supramolecular structures formed betweer the precursor molecules guided nanotube formation.The porous and nanotubular structure of the nanotubes facilitated efficient charge carrier nigration and separation,thereby enhancing photocatalytic Hz production in 20 vol.%lactic acid under visible light irradiation.Nanotubes synthesized using melamine and urea in a 1:10 mass ratio(denoted herein as CN-MU nanotubes)exhibited a photocatalytic hydroger production rate of 1,073.6μmol·h^-1·^-g with Pt as the cocatalyst,a rate of 4.7 and 3.1 times higher than traditional Pt/g-CN4 photocatalysts prepared from graphitic carbon nitride(g-CN4)obtained by direct thermal polymerization of melamine or urea,respectively.On the basis of their outstanding performance for photocatalytic H2 production,it is envisaged that the holey g-C3N4 nanotubes will find widespread uptake in other areas,including photocatalytic CO2 reduction,dye-sensitized solar cells and photoelectrochemical sensors.展开更多
Planar micro-supercapacitors （MSCs） have drawn extensive research attention owing to their unique structural design and size compatibility for microelectronic devices. Graphene has been widely used to improve the pe...Planar micro-supercapacitors （MSCs） have drawn extensive research attention owing to their unique structural design and size compatibility for microelectronic devices. Graphene has been widely used to improve the performance of microscale electrochemical capacitors. However, investigations of an intrinsic electrochemical mechanism for graphene-based microscale devices are still not sufficient. Here, micro-supercapacitors with various typical architectures are fabricated as models to study the graphene effect, and their electrochemical performance is also evaluated. The results show that ionic accessibility and adsorption are greatly improved after the introduction of the holey graphene intermediate layer. This study provides a new route to understand intrinsic electrochemical behaviors and possesses exciting potential for highly efficient on-chip micro-energy storage.展开更多
Efficient charge separation and rapid interfacial reaction kinetics are crucial factors that determine the efficiency of photocatalytic hydrogen evolution.Herein,a fascinating 2D heterojunction photocatalyst with supe...Efficient charge separation and rapid interfacial reaction kinetics are crucial factors that determine the efficiency of photocatalytic hydrogen evolution.Herein,a fascinating 2D heterojunction photocatalyst with superior photocatalytic hydrogen evolution performance–holey C_(3)N_(4)nanosheets nested with TiO_(2)nanocrystals(denoted as HCN/TiO_(2))–is designed and fabricated via an in situ exfoliation and conversion strategy.The HCN/TiO_(2)is found to exhibit an ultrathin 2D heteroarchitecture with intimate interfacial contact,highly porous structures and ultrasmall TiO_(2)nanocrystals,leading to drastically improved charge carrier separation,maximized active sites and the promotion of mass transport for photocatalysis.Consequently,the HCN/TiO_(2)delivers an impressive hydrogen production rate of 282.3 lmol h^(-1)per10 mg under AM 1.5 illumination and an apparent quantum efficiency of 13.4%at a wavelength of 420 nm due to the synergetic enhancement of surface reactions and charge separation.The present work provides a promising strategy for developing high-performance 2D heterojunctions for clean energy applications.展开更多
The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensional...The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensionally holey Pt nanotubes(Pt-hNTs)using Pt^(Ⅱ)-dimethylglyoxime complex(Pt^(Ⅱ)-DMG)nanorods as the reaction precursor.The coordination capability of DMG results in the generation of Pt^(Ⅱ)-DMG nanorods,whereas the reducibility of DMG at high temperature leads to the reduction of Pt^(Ⅱ)species in Pt^(Ⅱ)-DMG nanorods.During the reaction process,the inside-out Ostwald ripening phenomenon leads to the hollow morphology of Pt-hNTs.Benefiting from the physical characteristics of hollow and holey structure,Pt-hNTs with clean surface show superior electroactivity and durability for catalyzing ethanol electrooxidation as well as hydrogen evolution reaction in alkaline media.Under optimized experimental conditions,the constructed symmetric Pt-hNTs||Pt-hNTs ethanol electrolyzer only requires an electrolysis voltage of 0.40 V to achieve the electrochemical hydrogen production,demonstrating a highly energy saving strategy relative to traditional water electrolysis.展开更多
Fabricating electrodes with large specific surface area(SSA)and high permeability has been the longstanding target in redox flow batteries(RFBs).In this work,we propose a novel ZIF-8-assisted etching approach to form ...Fabricating electrodes with large specific surface area(SSA)and high permeability has been the longstanding target in redox flow batteries(RFBs).In this work,we propose a novel ZIF-8-assisted etching approach to form holey fibers in the electrospinning process of aligned electrode structures.The etching approach allows the formation of holey fibers with small pores of~50 nm,offering large active surface areas for redox reactions,while the aligned macrostructure with the holey fibers of 3–5 lm in diameter ensures a high permeability along the fiber direction.The application of the prepared electrodes to a vanadium redox flow battery(VRFB)enables an energy efficiency(EE)of 87.2%at the current density of 200 m A cm^(-2),which is 13.3%higher than that with conventional electrospun carbon electrodes.Even at high current densities of 300 and 400 m A cm^(-2),the battery still maintains energy efficiencies of 83.3%and 79.3%.More excitingly,the prepared electrode yields a high limiting current density of4500 m A cm^(-2) and a peak power density of 1.6 W cm^(-2).It is anticipated that the present electrospinning method combining the ZIF-8-assisted etching approach with a way to form ordered fiber structures will allow even more high-performance electrodes for RFBs in the future.展开更多
Nitrogen-doped graphene is a promising candidate for the replacement of noble metal-based electrocatalysts for oxygen reduction reactions （ORRs）. The addition of pores and holes into nitrogen-doped graphene enhances...Nitrogen-doped graphene is a promising candidate for the replacement of noble metal-based electrocatalysts for oxygen reduction reactions （ORRs）. The addition of pores and holes into nitrogen-doped graphene enhances the ORR activity by introducing abundant exposed edges, accelerating mass transfer, and impeding aggregation of the graphene sheets. Herein, we present a straightforward but effective strategy for generating porous holey nitrogen-doped graphene （PHNG） via the pyrolysis of urea and magnesium acetate tetrahydrate. Due to the combined effects of the in situ generated gases and MgO nanoparticles, the synthesized PHNGs featured not only numerous out-of-plane pores among the crumpled graphene sheets, but also interpenetrated nanoscale （5-15 nm） holes in the assembled graphene. Moreover, the nitrogen doping configurations of PHNG were optimized by post-thermal treatments at different temperatures. It was found that the overall content of pyridinic and quaternary nitrogen positively correlates with the ORR activity; in particular, pyridinic nitrogen generates the most desirable characteristics for the ORR. This work reveals new routes for the synthesis of PHNG-based materials and elucidates the contributions of various nitrogen species to ORRs.展开更多
The notion of a maximum distance holey packing is introduced and used to construct optimal ternary (n, 3, 3) codes for all lengths n≡2 (mod 3) and n≥8. Combining this with Etzion’s result, the existence problem for...The notion of a maximum distance holey packing is introduced and used to construct optimal ternary (n, 3, 3) codes for all lengths n≡2 (mod 3) and n≥8. Combining this with Etzion’s result, the existence problem for an optimal ternary (n, 3,3)code is solved completely.展开更多
Metal–organic frameworks(MOFs)with redox-active metal sites and controllable crystalline structures make it possible to access the merits of highly-efficient electrode materials in electrochemical energy storage syst...Metal–organic frameworks(MOFs)with redox-active metal sites and controllable crystalline structures make it possible to access the merits of highly-efficient electrode materials in electrochemical energy storage systems.However,most MOFs suffer from low capacitance and poor cycling stability that largely thwart their application.Herein,we present the holey graphene oxide(HGO)template strategy to prepare nano two-dimensional Ni(BDC)with HGO as both template and capping agent(denoted as Ni(BDC)-HGOx,x=10,20,30,and 40 according to the added HGO amount).Structural analyses reveal that HGO can significantly inhibit the Ni(BDC)agglomeration,thus offering a high ion-accessible surface area.Ni(BDC)-HGO30 with well-exposed active sites exhibits a high capacitance of 1,115.6 F·g^(−1) at 1 A·g^(−1) in 6 M KOH aqueous,1.8 times that of bulk Ni(BDC).An asymmetric supercapacitor with Ni(BDC)-HGO30 as a positive electrode and activated carbon as the opposing electrode delivers an energy density of 52.5 W·h·kg^(−1) and a power density up to 18.0 kW·kg−1,with 92.5%capacitance retention after 10,000 cycles.Galvanostatic intermittent titration technique and in situ electrochemical–Raman measurements were exploited to elucidate the electrochemical behavior of Ni(BDC)-HGO30.These results pave the way for the development of rationally tuned MOF materials for enhancing supercapacitor performances.展开更多
基金Funded by the National Natural Science Foundation of China(No.51972242)the National College Students'Innovation and Entrepreneurship Training Program(No.202210488020)+2 种基金the Open Fund of the Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steel making(Wuhan University of Science and Technology)of China(No.KF-20-5)the Research Project of Yingcheng Xinjincheng Environmental Protection Technology Co.,Ltd(No.2023420612000754)the Program(No.BG20210227001)of High-end Foreign Experts of the State of the State Administration of Foreign Experts Affairs(SAFEA)。
文摘In this study,the holey graphene was prepared by microwave-assisted chemical etching.The three-dimensional(3D)holey graphene hydrogel was obtained through hydrothermal self-assembly method,followed by the introduction of FeCo_(2)S_(4)particles.The resulting holey graphene hydrogel,characterized by high specific surface area and abundant pores combined with FeCo_(2)S_(4)with high pseudocapacitance by interfacial interaction,shortened the mass transport path and enhanced the specific capacitance.The findings reveal that the holey graphene hydrogel/FeCo_(2)S_(4)(FeCo_(2)S_(4)/HGH)composite exhibits high specific capacitance and impressive rate capability(413.4 F·g^(-1)at 1 A·g^(-1),300.4 F·g^(-1)at 6 A·g^(-1)).The symmetric supercapacitor operated within a stable potential window of 0.1-1.6 V,achieving specific capacitance of 127.5 F·g^(-1)at 1 A·g^(-1),and can deliver 37.1 Wh·kg^(-1)at a power density of 1499 W·kg^(-1).Besides,under the current density of 3 A·g^(-1),the supercapacitor retained 90.8%of its capacitance after 5000 cycles,demonstrating exceptional cycle stability.This study presents an efficient method for fabricating advanced integrated supercapacitors electrodes with enhanced energy density.
基金funded by the Ministry of Business,Innovation and Employment Endeavour Fund of New Zealand(MAUX1801)supported by the China Postdoctoral Science Foundation(2021M692622).
文摘An efficient chamber-induced activation method was applied for the preparation of holey graphene/cellulose nanofiber-based film with high specific surface area(SSA)and multiple channels through the graphene nanosheets.With the cellulose nanofiber(CNF)simultaneously serving as“dispersing agent,”“spacer,”and“activating agent,”the graphene oxide(GO)nanosheets are perforated by the pyrolysis gas from CNF in the confined space inside the hybrid films,uniformly dispersed,and sandwiched between CNF networks with less agglomeration and restacking.Additionally,we have proved that H2O and H2 are primarily responsible for the activation and etching of GO/CNF film.As the CNF content increases,the mesoporosity of the activated reduced GO/CNF(A-RGO/CNF)film increases,and the graphene nanosheets show more nanopore perforations.Benefitting from the high SSA,high density,moderate mesoporosity,and abundant channels for ion diffusion through the graphene nanosheets,the A-RGO/CNF film exhibits the highest specific capacitance of 323(236)F g^(−1)(F cm^(−3))at 1Ag^(−1).For the A-RGO5/CNF5 film containing half CNF and half GO,an excellent comprehensive electrochemical performance including superior rate performance(208(160)F g^(−1)(F cm^(−3))at 60Ag^(−1))is exhibited.Moreover,the A-RGO5/CNF5 electrode in an all-solid-state flexible symmetric supercapacitor delivers a high specific capacitance of 250(193)F g^(−1)(F cm^(−3))at 1Ag^(−1).This study provides a novel idea for the preparation of holey graphene-based film for supercapacitor electrodes.The strategy of simultaneously employing CNF as“dispersing agent,”“spacer,”and“activating agent”also offers a new vision for the assembly of homogeneous nanohybrid material and the utilization of pyrolysis gas.
文摘The oxygen evolution reaction(OER)is a half-reaction of water electrolysis,and the OER performance of an electrocatalyst is significantly related to its energy conversion efficiency.Due to their high OER activity,transition metal-based nanomaterials have become potential low-cost substitutes for Ir/Ru-based OER electrocatalysts in an alkaline environment.Herein,holey Fe3O4-coupled Ni(OH)2 sheets(Ni(OH)2-Fe H-STs)were easily achieved by a simple mixed-cyanogel hydrolysis strategy.The two-dimensional(2D)Ni(OH)2-Fe H-STs with ca.1 nm thickness have a high specific surface area,abundant unsaturated coordination atoms,and numerous pores,which are highly favorable for electrocatalytic reactions.Meanwhile,the introduction of Fe improves the conductivity and regulates the electronic structure of Ni.Due to their special structural features and synergistic effect between the Fe and Ni atoms,Ni(OH)2-Fe H-STs with an optimal Ni/Fe ratio show excellent OER activity in a 1 M KOH solution,which significantly exceeds that of the commercial RuO2 nanoparticle electrocatalyst.Furthermore,Ni(OH)2-Fe H-STs can be grown on nickel foam(NF),and the resulting material exhibits enhanced OER activity,such as a small overpotential of 200 mV and a small Tafel slope of 56 mV dec−1,than that of Ni(OH)2-Fe H-STs without NF.
基金financially supported by the National Key R&D Program of China (No.2017YFA0304203)the National Natural Science Foundation of China (Nos.21805174 and 51902190)+5 种基金the Key Research and Development Program of Shanxi Province for International Cooperation (No.201803D421082)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (Nos.2019L0013 and 2019L0018)Shanxi Scholarship Council of China (No.2021-004)the Program of Introducing Talents of Discipline to Universities (No.D18001)the Changjiang Scholars and Innovative Research Team at the University of Ministry of Education of China (No.IRT_17R70)the Fund for Shanxi “1331 Project”
文摘MXene has given great promises to superca-pacitor electrode material due to its high conductivity and redox properties.However,the self-agglomeration of the MXene lamella will reduce its contact area with the elec-trolyte and generate a tortuous transportation pathway of the electrolyte ions,thereby reducing its capacitive per-formance and rate capability.In this work,we engineered the electrolyte ion channels by adjusting the MXene lamella size and inserting holey graphene(HG)nanosheets into the interlayer of the MXene flakes.The developed MXene/HG electrode can not only avoid the self-restack-ing of MXene but also provide unimpeded ion transport channels.As a result,the supercapacitive and rate perfor-mances of the small MXene lamella-based MXene/HG(S-MXene/HG)supercapacitor are prominently ameliorated.By adjusting the content of HG,the S-MXene/HG0.05 electrode exhibits excellent gravimetric capacitance of 446 F·g^(-1)and a rate capability of 77.5%.The S-MXene/HG0.05-based symmetric supercapacitor provides an impressive energy density of 14.84 Wh·kg^(-1)with excellent cyclic stability of 96%capacitance retention after 10,000 cycles.This demonstration of the engineering of the ion channels shows great potential in two-dimensional mate-rial-based supercapacitor electrodes.
基金financially supported by the National Natural Science Foundation of China(No.52207249)the research program of Top Talent Project of Yantai University(No.1115/2220001)+1 种基金the Yantai Basic Research Project(No.2022JCYJ04)the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing(No.AMGM2021F11).
文摘Three-dimensional holey nitrogen-doped carbon matrixes decorated with molybdenum dioxide(MoO_(2))nanoparticles have been successfully synthesized via a NaCl-assisted template strategy.The obtained MoO_(2)/C composites offered multi-advantages,including higher specific surface area,more active sites,more ions/electrons transmission channels,and shorter transmission path due to the synergistic effect of the uniformly distributed MoO_(2) nanoparticles and porous carbon structure.Especially,the oxygen vacancies were introduced into the prepared composites and enhanced the Li^(+)intercalation/deintercalation process during electrochemical cycling by the Coulomb force.The existence of the local built-in electric field was proved by experimental data,differential charge density distribution,and density of states calculation.The uniquely designed structure and introduced oxygen vacancy defects endowed the MoO_(2)/C composites with excellent electrochemical properties.In view of the synergistic effect of the uniquely designed morphology and introduced oxygen vacancy defects,the MoO_(2)/C composites exhibited superior electrochemical performance of a high capacity of 918.2 mAh g^(-1) at 0.1 A g^(-1) after 130 cycles,562.1 mAh g^(-1) at 1.0 A g^(-1) after 1000 cycles,and a capacity of 181.25 mAh g^(-1) even at 20.0 A g^(-1).This strategy highlights the path to promote the commercial application of MoO_(2)-based and other transition metal oxide electrodes for energy storage devices.
基金financially supported by the National Natural Science Foundation of China (Nos.51872283,21805273)National Key R&D Program of China (Nos.2016YBF0100100, 2016YFA0200200)+5 种基金Liaoning BaiQianWan Talents ProgramLiaoNing Revitalization Talents Program (No.XLYC1807153)Natural Science Foundation of Liaoning Province,Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science (No. 20180510038)DICP (Nos.DICP ZZBS201708,DICP ZZBS201802)DICP&QIBEBT (No.DICP&QIBEBT UN201702)DNL Cooperation Fund,CAS (Nos.DNL180310,DNL180308,DNL201912,DNL201915)。
文摘Porous structure and heteroatom doping are two key parameters for significantly boosting the capacitive performance of graphene-based materials.Herein,we report a facile approach to prepare onedimensional(ID) nitrogen-doped holey graphene nanoscrolls(NHGNSs) through cold quenching treatment of two-dimensional graphene oxide sheets,followed by thermal annealing in the successive atmosphere of NH3 and air.Benefiting from the synergy of the unique 1D tubular morphology,abundant nanoholes and nitrogen doping,the NHGNSs exhibit a high specific capacitance of 126 F/g at 1 A/g in ionic liquid electrolyte and excellent rate capability with 81% of the capacitance retained at 20 A/g.Furthermore,the fabricated symmetric supercapacitors based on NHGNSs achieve both high energy density of 53.5 Wh/kg at 875 W/kg and high power density of 17.5 kW/kg at 43.4 Wh/kg.The simple synthetic process and superior electrochemical performance suggest the great potential of NHGNSs for supercapacitor application.
基金financial support from the“Young Talent Fellowship”program through South China University of Technologythe Fundamental Research Funds for the Central Universities(2018JQ06)。
文摘Lithium ion batteries(LIBs)have been widely used in portable and smart devices because of their high energy densities,long cycle life and environmental friendliness.In order to meet the evergrowing demand for human-beings utilizing electronic devices,electric vehicles and energy storage grids.
基金sponsored by the National Natural Science Foundation of China(22272103)the Natural Science Foundation of Shaanxi Province(2020JZ-23,2019KJXX-021,and 2020JM269)+7 种基金the Key Research and Development Program of Shaanxi(2020SF-355)the Science and Technology Innovation Team of Shaanxi Province(2022TD-35)the University Engineering Research Center of Crystal Growth and Applications of Guangdong Province(2020GCZX005)the Special Innovative Projects of Guangdong Province(2020KTSCX125)the Shenzhen Stable Supporting Program(SZWD2021015)the Fundamental Research Funds for the Central Universities(GK202202001)the Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials at Guangxi University(2021GXYSOF02)the 111 Project(B14041)。
文摘Both structure and interface engineering are highly effective strategies for enhancing the catalytic activity and selectivity of precious metal nanostructures.In this work,we develop a facile pyrolysis strategy to synthesize the high-quality holey platinum nanotubes(Pt-H-NTs)using nanorods-like Pt^(Ⅱ)-phenanthroline(PT)coordination compound as self-template and self-reduction precursor.Then,an up-bottom strategy is used to further synthesize polyallylamine(PA)modified Pt-H-NTs(Pt-HNTs@PA).PA modification sharply promotes the catalytic activity of Pt-H-NTs for the formic acid electrooxidation reaction(FAEOR)by the direct reaction pathway.Meanwhile,PA modification also elevates the catalytic activity of Pt-H-NTs for the hydrogen evolution reaction(HER)by the proton enrichment at electrolyte/electrode interface.Benefiting from the high catalytic activity of Pt-H-NTs@PA for both FAEOR and HER,a two-electrode FAEOR boosted water electrolysis system is fabricated by using Pt-H-NTs@PA as bifunctio nal electrocatalysts.Such FAEOR boosted water electrolysis system only requires the operational voltage of 0.47 V to achieve the high-purity hydrogen production,showing an energy-saving hydrogen production strategy compared to traditional water electrolysis system.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.60777031, 11074164)the Shanghai Leading Academic Discipline Project (Grant No.S30108)
文摘In order to design birefringent holey fiber with beat-length independent of wavelength, an asymmetric structure is introduced to reduce its wavelength-sensitivity. The influence of structural parameters on the modal birefringence is calculated and analyzed. After optimizing the parameters, a flat dispersion curve of beat-length is obtained. The beat-length changes from 89.8 mm to 91.0 mm in wavelength range from 1.1 μm, to 1.7μm, and its relative variation is 1.38%. If this fiber is made into zero-order quarter wave plate, the phase delay can be easily controlled in （90±1）°.
文摘The high power holey fiber is an efficient supercontinuum light source by using picosecond pulse,which is a less expensive laser source compared with low power and expensive femtosecond laser sources. In this paper, a high power highly nonlinear holey fiber(HN-HF) with a low confinement loss is proposed for supercontinuum light sources. The finite difference method is used to calculate the different properties of the proposed HN-HF. High nonlinear coefficients are obtained at 1.06 μm, 1.31μm, and 1.55μm wavelengths with flattened chromatic dispersion and low confinement losses simultaneously. Moreover, numerical simulation results show that high power broad supercontinuum spectra with very short length of the proposed photonic crystal fiber are achieved.
基金Project supported by the National Natural Science Foundation of China (Grant No. 10874145)Specialized Research Fund for the Doctoral Program of Higher Education (Grant No. 20091333110010)+1 种基金the Natural Science Foundation of Hebei Province of China (Grant No. F2009000481)the China Postdoctoral Science Foundation (Grant Nos. 20080440014 and 200902046)
文摘This paper proposes three kinds of tapered holey fibres with a multi-layer of holes whose pitch of air holes at the end of untapered and tapered are 5.8 μm and 1.8 μm. The central wavelength which locates in the anomalous dispersion region is 1.55 μm. An adaptive split-step Fourier method is numerically used to study the pulse propagation in tapered holey fibres. For the considered convex tapered holey fibre, at a wavelength of 1.55 μm, a compression factor of 136.7 can be achieved by initial width of 800 fs propagation through a length of 0.8 m. It demonstrates that in anomalous dispersion region, pulse can be compressed with the increase of nonlinearity coefficient and the decrease of dispersion coefficient.
基金Institute of Information Communications Technology Planning Evaluation(2022-0-01029,RS-2022-II221044)National Research Foundation(2023R1A2C1007165)。
文摘In this study,we introduce and experimentally validate,to our knowledge,a new type of terahertz(THz)fiber waveguide.The waveguide features a core made from petroleum jelly(commonly known as Vaseline)and a cladding made of holey polytetrafluoroethylene(PTFE),also known as Teflon.Since the core is biocompatible and the cladding is safe for human use,this design has promising applications for biocompatible probes in the THz range.We rigorously analyzed the transmission properties of the waveguide using the finite element method(FEM)and followed up with experimental validation using a THz time-domain spectroscopy(THz-TDS)system.The fiber supports single-mode operation for frequencies below 0.9 THz and demonstrates low-loss transmission of THz waves,even when tightly bent.For instance,with a bending radius as small as 1.61 cm,the fiber exhibited minimal losses of 0.23 dB/cm at 0.2 THz and 0.27 dB/cm at 0.5 THz,surpassing previous technical limitations.Another key advantage is the strong confinement of the THz waves within the petroleum jelly core,which helps maintain low dispersion and ensures stable pulse transmission,even under tight bends.The exceptional stability and flexibility of this biocompatible THz fiber make it highly suitable for sensing and imaging applications in confined,flexible environments,including potential uses within the human body.
基金The authors are grateful for the financial support from the National Key R&D Program of China(Nos.2018YFB1502002,2017YFA0206904,2017YFA0206900,and 2016YFB0600901)the National Natural Science Foundation of China(Nos.51825205,U1662U&51772305,51572270,21871279,and 21802154)+4 种基金the Beijing Natural Science Foundation(Nos.2191002,218207&and 2194089)the Beijing Municipal Science and Technology Project(No.Z181100005118007)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)the Royal Society-Newton Advanced Fellowship(No.NA170422)the International Partnership Program of Chinese Academy of Sciences(No.GJHZ1819)and the K.C.Wong Education Foundation.G.I.N.W.acknowledges funding support from the Energy Education Trust of New Zealand and the University of Auckland Faculty Research Development Fund.
文摘A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes,involving direci eating of mixtures of melamine and urea or melamine and cyanuric acid in specific mass ratios.Supramolecular structures formed betweer the precursor molecules guided nanotube formation.The porous and nanotubular structure of the nanotubes facilitated efficient charge carrier nigration and separation,thereby enhancing photocatalytic Hz production in 20 vol.%lactic acid under visible light irradiation.Nanotubes synthesized using melamine and urea in a 1:10 mass ratio(denoted herein as CN-MU nanotubes)exhibited a photocatalytic hydroger production rate of 1,073.6μmol·h^-1·^-g with Pt as the cocatalyst,a rate of 4.7 and 3.1 times higher than traditional Pt/g-CN4 photocatalysts prepared from graphitic carbon nitride(g-CN4)obtained by direct thermal polymerization of melamine or urea,respectively.On the basis of their outstanding performance for photocatalytic H2 production,it is envisaged that the holey g-C3N4 nanotubes will find widespread uptake in other areas,including photocatalytic CO2 reduction,dye-sensitized solar cells and photoelectrochemical sensors.
基金This work was supported by the National Basic Research Program of China （Nos. 2013CB934103 and 2012CB933003）, the International Science ＆ Technology Cooperation Program of China （No. 2013DFA50840）, the National Natural Science Foundation of China （Nos. 51522001 and 51272197）, the National Science Fund for Hubei Provincial Natural Science Young Scholars （No. 51425204）, the Hubei Science Fund for Distinguished Young Scholars （No. 2014CFA035）, the Fundamental Research Funds for the Central Universities （WUT： 2015-PY-2, 2015-CL-A1-03）. We are deeply thankful to Prof. Charles M. Lieber of Harvard University, Prof. Dongyuan Zhao of Fudan University, and Prof. Jun Liu of Pacific Northwest National Laboratory for their stimulating discussion and kind help.
文摘Planar micro-supercapacitors （MSCs） have drawn extensive research attention owing to their unique structural design and size compatibility for microelectronic devices. Graphene has been widely used to improve the performance of microscale electrochemical capacitors. However, investigations of an intrinsic electrochemical mechanism for graphene-based microscale devices are still not sufficient. Here, micro-supercapacitors with various typical architectures are fabricated as models to study the graphene effect, and their electrochemical performance is also evaluated. The results show that ionic accessibility and adsorption are greatly improved after the introduction of the holey graphene intermediate layer. This study provides a new route to understand intrinsic electrochemical behaviors and possesses exciting potential for highly efficient on-chip micro-energy storage.
基金the National Key R&D Program of China(2018YFE0201704 and 2018YFE0201701)the National Natural Science Foundation of China(21673256,21533011,2163100,and 21603036)Shanghai Rising-Star Program.
文摘Efficient charge separation and rapid interfacial reaction kinetics are crucial factors that determine the efficiency of photocatalytic hydrogen evolution.Herein,a fascinating 2D heterojunction photocatalyst with superior photocatalytic hydrogen evolution performance–holey C_(3)N_(4)nanosheets nested with TiO_(2)nanocrystals(denoted as HCN/TiO_(2))–is designed and fabricated via an in situ exfoliation and conversion strategy.The HCN/TiO_(2)is found to exhibit an ultrathin 2D heteroarchitecture with intimate interfacial contact,highly porous structures and ultrasmall TiO_(2)nanocrystals,leading to drastically improved charge carrier separation,maximized active sites and the promotion of mass transport for photocatalysis.Consequently,the HCN/TiO_(2)delivers an impressive hydrogen production rate of 282.3 lmol h^(-1)per10 mg under AM 1.5 illumination and an apparent quantum efficiency of 13.4%at a wavelength of 420 nm due to the synergetic enhancement of surface reactions and charge separation.The present work provides a promising strategy for developing high-performance 2D heterojunctions for clean energy applications.
基金supported by the Natural Science Foundation of Hainan Province(2019RC007)Key Research and Development Project of Hainan Province(ZDYF2020037)+5 种基金the National Natural Science Foundation of China(21875133 and 51873100)Natural Science Foundation of Shaanxi Province(2020JZ-23)Fundamental Research Funds for the Central Universities(GK202101005,GK201901002,2019TS007,2021CBLZ004,and 2020CSLZ012)the Innovation Team Project for Graduate Students at Shaanxi Normal University(TD2020048Y)Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials at Guangxi University(2021GXYSOF02)the 111 Project(B14041)。
文摘The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensionally holey Pt nanotubes(Pt-hNTs)using Pt^(Ⅱ)-dimethylglyoxime complex(Pt^(Ⅱ)-DMG)nanorods as the reaction precursor.The coordination capability of DMG results in the generation of Pt^(Ⅱ)-DMG nanorods,whereas the reducibility of DMG at high temperature leads to the reduction of Pt^(Ⅱ)species in Pt^(Ⅱ)-DMG nanorods.During the reaction process,the inside-out Ostwald ripening phenomenon leads to the hollow morphology of Pt-hNTs.Benefiting from the physical characteristics of hollow and holey structure,Pt-hNTs with clean surface show superior electroactivity and durability for catalyzing ethanol electrooxidation as well as hydrogen evolution reaction in alkaline media.Under optimized experimental conditions,the constructed symmetric Pt-hNTs||Pt-hNTs ethanol electrolyzer only requires an electrolysis voltage of 0.40 V to achieve the electrochemical hydrogen production,demonstrating a highly energy saving strategy relative to traditional water electrolysis.
基金financially supported by the grant from the Research Grants Council of the Hong Kong Special Administrative Region,China(T23-601/17-R)the National Natural Science Foundation of China(21703263)HKUST Fund of Nanhai(FSNH-18FYTRI01)。
文摘Fabricating electrodes with large specific surface area(SSA)and high permeability has been the longstanding target in redox flow batteries(RFBs).In this work,we propose a novel ZIF-8-assisted etching approach to form holey fibers in the electrospinning process of aligned electrode structures.The etching approach allows the formation of holey fibers with small pores of~50 nm,offering large active surface areas for redox reactions,while the aligned macrostructure with the holey fibers of 3–5 lm in diameter ensures a high permeability along the fiber direction.The application of the prepared electrodes to a vanadium redox flow battery(VRFB)enables an energy efficiency(EE)of 87.2%at the current density of 200 m A cm^(-2),which is 13.3%higher than that with conventional electrospun carbon electrodes.Even at high current densities of 300 and 400 m A cm^(-2),the battery still maintains energy efficiencies of 83.3%and 79.3%.More excitingly,the prepared electrode yields a high limiting current density of4500 m A cm^(-2) and a peak power density of 1.6 W cm^(-2).It is anticipated that the present electrospinning method combining the ZIF-8-assisted etching approach with a way to form ordered fiber structures will allow even more high-performance electrodes for RFBs in the future.
基金Acknowledgements We gratefully acknowledge the financial support from the National Natural Science Foundation of China （Nos. 21503253, 21403276 and 91545109）, Natural Science Foundation of Shan-Xi province of China （No. 2015011010）, and Youth Innovation Promotion Association CAS （No. 2015141）.
文摘Nitrogen-doped graphene is a promising candidate for the replacement of noble metal-based electrocatalysts for oxygen reduction reactions （ORRs）. The addition of pores and holes into nitrogen-doped graphene enhances the ORR activity by introducing abundant exposed edges, accelerating mass transfer, and impeding aggregation of the graphene sheets. Herein, we present a straightforward but effective strategy for generating porous holey nitrogen-doped graphene （PHNG） via the pyrolysis of urea and magnesium acetate tetrahydrate. Due to the combined effects of the in situ generated gases and MgO nanoparticles, the synthesized PHNGs featured not only numerous out-of-plane pores among the crumpled graphene sheets, but also interpenetrated nanoscale （5-15 nm） holes in the assembled graphene. Moreover, the nitrogen doping configurations of PHNG were optimized by post-thermal treatments at different temperatures. It was found that the overall content of pyridinic and quaternary nitrogen positively correlates with the ORR activity; in particular, pyridinic nitrogen generates the most desirable characteristics for the ORR. This work reveals new routes for the synthesis of PHNG-based materials and elucidates the contributions of various nitrogen species to ORRs.
基金Project supported by the National Natural Science Foundation of China (Grant No. 19671064)
文摘The notion of a maximum distance holey packing is introduced and used to construct optimal ternary (n, 3, 3) codes for all lengths n≡2 (mod 3) and n≥8. Combining this with Etzion’s result, the existence problem for an optimal ternary (n, 3,3)code is solved completely.
基金supported by the National Natural Science Foundation of China(Nos.22105226 and 51972342)the Shandong Province Postdoctoral Innovative Talent Support Program(No.SDBX20200004)+3 种基金the China Postdoctoral Science Foundation(No.2020M682253)the Qingdao Postdoctoral Funding Project(No.ZX20210067)he Independent innovation scientific research project(No.20CX06100A)the Taishan Scholar Project of Shandong Province(No.ts20190922).
文摘Metal–organic frameworks(MOFs)with redox-active metal sites and controllable crystalline structures make it possible to access the merits of highly-efficient electrode materials in electrochemical energy storage systems.However,most MOFs suffer from low capacitance and poor cycling stability that largely thwart their application.Herein,we present the holey graphene oxide(HGO)template strategy to prepare nano two-dimensional Ni(BDC)with HGO as both template and capping agent(denoted as Ni(BDC)-HGOx,x=10,20,30,and 40 according to the added HGO amount).Structural analyses reveal that HGO can significantly inhibit the Ni(BDC)agglomeration,thus offering a high ion-accessible surface area.Ni(BDC)-HGO30 with well-exposed active sites exhibits a high capacitance of 1,115.6 F·g^(−1) at 1 A·g^(−1) in 6 M KOH aqueous,1.8 times that of bulk Ni(BDC).An asymmetric supercapacitor with Ni(BDC)-HGO30 as a positive electrode and activated carbon as the opposing electrode delivers an energy density of 52.5 W·h·kg^(−1) and a power density up to 18.0 kW·kg−1,with 92.5%capacitance retention after 10,000 cycles.Galvanostatic intermittent titration technique and in situ electrochemical–Raman measurements were exploited to elucidate the electrochemical behavior of Ni(BDC)-HGO30.These results pave the way for the development of rationally tuned MOF materials for enhancing supercapacitor performances.
