Lithium-sulfur(Li-S)batteries,although a promising candidate of next-generation energy storage devices,are hindered by some bottlenecks in their roadmap toward commercialization.The key challenges include solving the ...Lithium-sulfur(Li-S)batteries,although a promising candidate of next-generation energy storage devices,are hindered by some bottlenecks in their roadmap toward commercialization.The key challenges include solving the issues such as low utilization of active materials,poor cyclic stability,poor rate performance,and unsatisfactory Coulombic efficiency due to the inherent poor electrical and ionic conductivity of sulfur and its discharged products(e.g.,Li2S2 and Li_(2)S),dissolution and migration of polysulfide ions in the electrolyte,unstable solid electrolyte interphase and dendritic growth on an odes,and volume change in both cathodes and anodes.Owing to the high specific surface area,pore volume,low density,good chemical stability,and particularly multimodal pore sizes,hierarchical porous carbon(HPC)mate rials have received considerable attention for circumventing the above pro blems in Li-S batteries.Herein,recent progress made in the synthetic methods and deployment of HPC materials for various components including sulfur cathodes,separators and interlayers,and lithium anodes in Li-S batteries is presented and summarized.More importantly,the correlation between the structures(pore volume,specific surface area,degree of pores,and heteroatom-doping)of HPC and the electrochemical performances of Li-S batteries is elaborated.Finally,a discussion on the challenges and future perspectives associated with HPCs for Li-S batteries is provided.展开更多
Lithium-selenium(Li-Se)batteries have attracted considerable attentions for next-generation energy storage systems owing to high volumetric capacity of 3265 m Ah cm^(-3) and excellent electronic conductivity(~10^(-5)S...Lithium-selenium(Li-Se)batteries have attracted considerable attentions for next-generation energy storage systems owing to high volumetric capacity of 3265 m Ah cm^(-3) and excellent electronic conductivity(~10^(-5)S cm^(-1))of selenium.However,the shuttling effect and capacity fading prevent their wide applications.Herein we report a low-cost strategy for scalable fabrication of lignin derived hierarchical porous carbon(LHPC)as a new high-loading Se host for high-capacity and long-term cycling Li-Se batteries in carbonate electrolyte.The resulting LHPC exhibits three-dimensional(3D)hierarchically porous structure,high specific surface area of 1696 m^(2) g^(-1),and hetero-atom doping(O,S),which can effectively confine the Se particles into the micropores,and meanwhile,offer effective chemical binding sites for selenides from hetero-atoms(O,S).As a result,our Li-Se batteries based on Se@LHPC demonstrate high capacity of 450 m Ah g^(-1) at 0.5 C after 500 cycles,with a low capacity fading rate of only 0.027%.The theoretical simulation confirmed the strong affinity of selenides on the O and S sites of LHPC effectively mitigating the Se losing.Therefore,our strategy of using lignin as the low-cost precursor of hierarchically porous carbon for high-loading Se host offers new opportunities for high-capacity and long-life Li-Se batteries.展开更多
Self-aggregation and sluggish transport kinetics of cathode materials would usually lead to the poor electrochemical performance for aqueous zinc-ion batteries(AZIBs).In this work,we report the construction of C@VO_(2...Self-aggregation and sluggish transport kinetics of cathode materials would usually lead to the poor electrochemical performance for aqueous zinc-ion batteries(AZIBs).In this work,we report the construction of C@VO_(2) composite via anti-aggregation growth and hierarchical porous carbon encapsulation.Both of the morphology of composite and pore structure of carbon layer can be regulated by tuning the adding amount of glucose.When acting as cathode applied for AZIBs,the C@VO_(2)-3:3 composite can deliver a high capacity of 281 m Ah g^(-1) at 0.2 A g^(-1).Moreover,such cathode also exhibits a remarkably rate capability and cyclic stability,which can release a specific capacity of 195 m Ah g^(-1) at 5 A g^(-1) with the capacity retention of 95.4%after 1000 cycles.Besides that,the evolution including the crystal structure,valence state and transport kinetics upon cycling were also deeply investigated.In conclusion,benefited from the synergistic effect of anti-aggregation morphology and hierarchical porous carbon encapsulation,the building of such C@VO_(2) composite can be highly expected to enhance the ion accessible site,boost the transport kinetics and thus performing a superior storage performance.Such design concept can be applied for other kinds of electrode materials and accelerating the development of highperformance AZIBs.展开更多
Room temperature sodium-sulfur(RT Na-S)batteries are gaining extensive attention as attractive alternatives for large-scale energy storage,due to low cost and high abundancy of sodium and sulfur in nature.However,the ...Room temperature sodium-sulfur(RT Na-S)batteries are gaining extensive attention as attractive alternatives for large-scale energy storage,due to low cost and high abundancy of sodium and sulfur in nature.However,the dilemmas regarding soluble polysulfides(Na_(2)Sn,4<n<8)and the inferior reaction kinetics limit their practical application.To address these issues,we report the activated porous carbon fibers(APCF)with small sulfur molecules(S2-4)confined in ultramicropores,to achieve a reversible single-step reaction in RT Na-S batteries.The mechanism is investigated by the in situ UV/vis spectroscopy,which demonstrates Na2S is the only product during the whole discharge process.Moreover,the hierarchical carbon structure can enhance areal sulfur loading without sacrificing the capacity due to thorough contact between electrolyte and sulfur electrode.As a consequence,the APCF electrode with 38 wt%sulfur(APCF-38S)delivers a high initial reversible specific capacity of 1412 mAh g^(-1) and 10.6mAh cm^(-2)(avg.areal sulfur loading:7.5 mg cm^(-2))at 0.1 C(1C=1675 mA g^(-1)),revealing high degree of sulfur utilization.This study provides a new strategy for the development of high areal capacity RT Na-S batteries.展开更多
Hierarchical porous carbon material(MMC)was successfully fabricated via hard template synthesis method by carbonization of furfury alcohol within the template(MCM-41).The prepared MMC was studied with characterization...Hierarchical porous carbon material(MMC)was successfully fabricated via hard template synthesis method by carbonization of furfury alcohol within the template(MCM-41).The prepared MMC was studied with characterization methods including scanning electron microscopy(SEM),transmission electron microscopy(TEM),nitrogen adsorption-desorption analyses,and infrared spectral analysis(FTIR).To investigate kinetics of toluene adsorption of hierarchical porous carbon materials,the adsorption performances of these carbon samples with varying pore structure(MC-1,MMC,MMHPC)were analyzed via dynamic adsorption.And the Langmuir model and Freundlich equation were employed to correspond with adsorption isotherms to study the adsorption mechanism.The experimental results demonstrate that the Langmuir model is more appropriate to describe the adsorption process.The capacities of toluene adsorption follow the order of MMC<MMHPC(micro-meso hierarchical porous carbon)<MC-1(microporous carbon).MC-1 has satisfactory absorption performance due to its large pore volume and high ratio of micropores.MMHPC has excellent toluene adsorption performance for proper amounts of surface oxygen containing groups.Long saturation time,interconnected hierarchical pore channels,and large specific surface area make MMC also a promising material for VOCs treatment.These data reveal that the pore channel structure,rational pore distribution,high surface area and reasonable amounts of surface oxygen groups are the main factors contributed to excellent toluene adsorption performance,which proposes theoretical basis for hierarchical porous carbon materials to further engineering application.展开更多
Fossil fuel exhaustion and overdevelopment usually lead to a recession,which is worsened by the environmental pollution.So it is of high priority to develop high-efficiency energy storage device.Here,agreen and enviro...Fossil fuel exhaustion and overdevelopment usually lead to a recession,which is worsened by the environmental pollution.So it is of high priority to develop high-efficiency energy storage device.Here,agreen and environment-friendly strategy is devised to fabricate carbon materials from biomass.By water extraction and alcohol precipitation,polysaccharide is extracted from loquat leaves.After calcining under high temperature,hierarchical porous carbon materials(HPCM)are obtained,possessing a variety of macropores,mesopores and micropores.Such ample and hierarchical pores enable the electrolyte infiltration and the buffering of the volume expansion of sulfur in repeated electrochemical reactions.The structure stability of the entire electrode can thus be well maintained.When evaluated as the scaffold for sulfur,the electrochemical performance of carbon/sulfur composite was tested.Even after 500 cycles,the reversible capacity is retained as high as 485.4 mA·h/g at the current density of 1.6 A/g.It also offers a notable rate capability,attaining the discharge capacity of 700.7 mA·h/g at 2 C.All the electrochemical performance results prove the feasibility of the proposed strategy.展开更多
Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed ...Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.展开更多
Dual heteroatom-doped carbons have attracted widespread research attention as catalysts in the field of energy storage and conversion due to their unique electronic structures and chemical tunability.In particular,bor...Dual heteroatom-doped carbons have attracted widespread research attention as catalysts in the field of energy storage and conversion due to their unique electronic structures and chemical tunability.In particular,boron and nitrogen co-doped carbon(B,N@C)has shown great potential for photo/electrocatalytic applications.However,more needs to be done for rational designing and regulating the structure of these materials to improve their catalytic performance.Herein,monodispersed hierarchical porous B,N@C nanocages were fabricated by pyrolyzing zeolite imidazole framework(ZIF)which was treated with ammonia borane or boric acid via an integrated double-solvent impregnation and nanocofined-etching method.The treated ZIF-8 provided an essential structural template to achieve B,N co-doped hierarchical structures with micro/meso/macro multimodal pore size distributions.The resultant B,N@C nanocages displayed high catalytic activities for electrochemical oxygen reduction reaction(ORR)in alkaline media,outperforming most carbon-based catalysts,particularly from the perspective of the half-wave potentials.Such high catalytic performance is due to the enhanced activity by the coexistence of B and N and the mass transfer promoted by the unique hierarchical porous structure.展开更多
In this work,hydrothermal technique combined with KOH activation were employed to develop a series of porous carbons (NPCK-x) using tobacco stem as a low-cost carbon source and (NH_(4))_(2)C_(2)O_(4)as a novel nitroge...In this work,hydrothermal technique combined with KOH activation were employed to develop a series of porous carbons (NPCK-x) using tobacco stem as a low-cost carbon source and (NH_(4))_(2)C_(2)O_(4)as a novel nitrogen-doping agent.Physicochemical properties of NPCK-x were characterized by Brunauer-Emmett-Teller,field emission scanning electron microscopy,X-ray diffraction,Raman microscope,elemental analysis,and X-ray photoelectron spectroscopy.Results showed that the NPCK-x samples possessed large surface areas (maximum:2875 m^(2)/g),hierarchical porous structures,and high degree of disorder.N-containing functional groups decomposed during activation process,which could be the dominant reason for appearance of abundant mesopores and well-developed pore structure.Dynamic chlorobenzene adsorption experiments demonstrated that carbon materials with(NH_(4))_(2)C_(2)O_(4)modification exhibited higher adsorption capacity (maximum:1053 mg/g) than those without modification (maximum:723 mg/g).The reusability studies of chlorobenzene indicated that the desorption efficiency of (NH_(4))_(2)C_(2)O_(4)modified porous carbon reached90.40%after thermal desorption at 100℃ under N2atmosphere.Thomas model fitting results exhibited that the existence of mesopores accelerated the diffusion rate of chlorobenzene in porous carbon.Moreover,Grand Canonical Monte Carlo simulation was conducted to verify that micropores with pore sizes of 1.2–2 nm of the optimized porous carbon were the best adsorption sites for chlorobenzene and mesopores with pore sizes of 2–5 nm were also highly active sites for chlorobenzene adsorption.展开更多
The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the explorat...The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts.展开更多
The hierarchically porous carbons (HPCs) were prepared by sol-gel selassembly technology in different surfactant concentrations and were used as the potential electrode for lithium oxygen batteries. The physical and...The hierarchically porous carbons (HPCs) were prepared by sol-gel selassembly technology in different surfactant concentrations and were used as the potential electrode for lithium oxygen batteries. The physical and electrochemical properties of the as-prepared HPCs were investigated by filed emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), nitrogen adsorption-desorption isotherm and galvanostatic charge/discharge. The results indicate that all of the HPCs mainly possess mesoporous structure with nearly similar pore size distribution. Using the HPCs as the electrode, a high discharge capacity for lithium oxygen battery can be achieved, and the discharge capacity increases with the specific surface area. Especially, the HPCs-3 oxygen electrode with CTAB concentration of 0.27 mol/L exhibits good capacity retention through controlling discharge depth to 800 mA·h/g and the highest discharge capacity of 2050 mA·h/g at a rate of 0.1 mA/cm2.展开更多
Sodium-ion batteries (SIBs) have been attracting considerable attention as a promising candidate for large-scale energy storage because of the abundance and low-cost of sodium resources. However, lack of appropriate a...Sodium-ion batteries (SIBs) have been attracting considerable attention as a promising candidate for large-scale energy storage because of the abundance and low-cost of sodium resources. However, lack of appropriate anode materials impedes further applications. Herein, a novel self-template strategy is designed to synthesize uniform flowerlike N-doped hierarchical porous carbon networks (NHPCN) with high content of N (15.31 at.%) assembled by ultrathin nanosheets via a self-synthesized single precursor and subsequent thermal annealing. Relying on the synergetic coordination of benzimidazole and 2-methylimidazole with metal ions to produce a flowerlike network, a self-formed single precursor can be harvested. Due to the structural and compositional advantages, including the high N doping, the expanded interlayer spacing, the ultrathin two-dimensional nano-sized subunits, and the three-dimensional porous network structure, these unique NHPCN flowers deliver ultrahigh reversible capacities of 453.7 mAh·g^−1 at 0.1 A·g^−1 and 242.5 mAh·g^−1 at 1 A·g^−1 for 2,500 cycles with exceptional rate capability of 5 A·g^−1 with reversible capacities of 201.2 mAh·g^−1. The greatly improved sodium storage performance of NHPCN confirms the importance of reasonable engineering and synthesis of hierarchical carbon with unique structures.展开更多
Advanced zinc-cerium redox flow battery(ZCRFB) is a large-scale energy storage system which plays a significant role in the application of new energy sources. The requirement of superior cathode with high acitivity ...Advanced zinc-cerium redox flow battery(ZCRFB) is a large-scale energy storage system which plays a significant role in the application of new energy sources. The requirement of superior cathode with high acitivity and fast ion diffusion is a hierarchical porous structure, which was synthesized in this work by a method in which both hard template and soft template were used. The structure and the performance of the cathode prepared here were characterized and evaluated by a variety of techniques such as scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray photoelectron spectroscopy(XPS), cyclic voltammetry(CV), linear sweep voltammetry(LSV), and chronoamperometry(CA). There were mainly three types of pore size within the hierarchical porous carbon: 2 μm, 80 nm, and 10 nm. The charge capacity of the cell using hierarchical porous carbon(HPC) as positive electrode was obviously larger than that using carbon felt; the former was 665.5 mAh with a coulombic efficiency of 89.0% and an energy efficiency of 79.0%, whereas the latter was 611.1 mAh with a coulombic efficiency of 81.5% and an energy efficiency of 68.6%. In addition, performance of the ZCRFB using HPC as positive electrode showed a good stability over 50 cycles.These results showed that the hierarchical porous carbon was superior over the carbon felt for application in ZCRFB.展开更多
Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth proces...Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth process of lithium sulfide leads to a thick insulating film covering the electrode, inducing slow electrons transfer and mass-transfer of ions and liquid sulfur species in working Li-S cells. Here, we demonstrate a bio-inspired strategy of constructing ant-nest-like hierarchical porous ultrathin carbon nanosheet networks with the implants of metallic nanoparticles electrocatalysts (HPC-MEC) as efficient nanoreactors enabling rapid mass transfer, via a simple and green NaCl template. Such nanoreactors with a large active surface area could effectively anchor polysulfides for mitigating the shuttle effect, facilitating uniformly thin Li2S film, and promoting the mass transfer for fast sulfur species conversions. This helps contribute to a continuously high sulfur utilization in Li-S batteries with the HPC-MEC reactors. As a typical exhibition, cobalt embedded hierarchical porous carbon (HPC-Co) could realize to deliver a remarkably high specific capacity of 1,540.6 mAh·g−1, an excellent rate performance of 878.8 mAh·g−1 at 2 C, and high area capacity of 11.6 mAh·cm−2 at a high sulfur load of 10 mg·cm−2 and low electrolyte/sulfur ratio of 5 µL·mg−1.展开更多
A novel synthesis of hierarchical porous carbons (HPCs)with 3D open-cell structure based on nanosilica- embedded emulsion-templated polymerization was reported. An oil-in-water emulsion containing SiO2 colloids was ...A novel synthesis of hierarchical porous carbons (HPCs)with 3D open-cell structure based on nanosilica- embedded emulsion-templated polymerization was reported. An oil-in-water emulsion containing SiO2 colloids was fabricated using liquid paraffin as an oil phase, resorcinol/formaldehyde and silica sol as an aqueous phase, and Span 80/Tween 80 as emulsifiers. HPCs with macropore cores, open meso/ macropore windows, and abundant micropores were synthesized by the polymerization and carbonization of the emulsion, followed by scaffold removal and further KOH activation. A typical HPCs sample as supercapacitor electrode shows the charge/discharge capability under large loading current density (30 A/g) coupling with a reasonable electrochemical capacitance in KOH electrolyte solution.展开更多
Large surface area,high conductivity,and rich active site of carbon electrode materials are necessary characteristics for energy storage devices.However,high conductivity and high nitrogen doping of carbon electrode m...Large surface area,high conductivity,and rich active site of carbon electrode materials are necessary characteristics for energy storage devices.However,high conductivity and high nitrogen doping of carbon electrode materials are difficult to coordinate.Here,a facile method via the carbonization of nitrogen-containing Schiff base polymer has been developed to prepare high conductivity and high nitrogen-doped hierarchical porous carbon.The organic components with a benzene ring structure in the polymer promote the formation of more sp^(2)-graphitized carbon,which is beneficial for the improvement of electrical conductivity.Nitrogen-doped hierarchical porous carbon calcined at 900℃ under the NH3 atmosphere possesses high nitrogen content of 7.48 at%,a large specific surface area of 1613.2m2/g,and high electrical conductivity of 2.7 S/cm.As electrode materials in an aqueous-based supercapacitor,nitrogen-doped hierarchical porous carbon exhibits superior specific capacitance of 385 F/g at 1 A/g as well as excellent rate performance(242 and 215 F/g at a current density of 100 and 200 A/g,respectively).In addition,the specific capacitance of electrode measured in a two-electrode system is 335 F/g at 1 A/g,and the long-term cycling stability can be achieved with more than 94%initial capacitance after 10000 cycles.The constructed symmetric supercapacitor delivers high energy density and high power density.The outstanding electrochemical performances combined with the novel and scalable synthetic approach make the nitrogen‐doped hierarchical porous carbon potential electrode material for electrochemical devices.展开更多
Hierarchical porous carbon(HPC)from bituminous coal was designed and synthesized through pyrolysis foaming and KOH activation.The obtained HPC(NCF-KOH)were characterized by a high specific surface area(S_(BET))of 3472...Hierarchical porous carbon(HPC)from bituminous coal was designed and synthesized through pyrolysis foaming and KOH activation.The obtained HPC(NCF-KOH)were characterized by a high specific surface area(S_(BET))of 3472.41 m^(2)/g,appropriate mesopores with V_(mes)/V_(total)of 57%,and a proper amount of surface oxygen content(10.03%).This NCF-KOH exhibited a high specific capacitance of 487 F/g at 1.0 A/g and a rate capability of 400 F/g at 50 A/g based on the three-electrode configuration.As an electrode for a symmetric capacitor,a specific capacitance of 299 F/g at 0.5 A/g was exhibited,and the specific capacitance retained 96%of the initial capacity at 5 A/g after 10,000 cycles.Furthermore,under the power density of 249.6 W/kg in 6 mol/L KOH,a high energy density of 10.34 Wh/kg was obtained.The excellent charge storage capability benefited from its interconnected hierarchical pore structure with high accessible surface area and the suitable amount of oxygen-containing functional groups.Thus,an effective strategy to synthesize HPC for high-performance supercapacitors serves as a promising way of converting coal into advanced carbon materials.展开更多
We report a convenient method to synthesize O,N-codoped hierarchical porous carbon by one-step carbonization of the mixture of KHCO3,urea and alginic acid.Benefiting from KHCO3 and urea syne rgistic effect,the obtaine...We report a convenient method to synthesize O,N-codoped hierarchical porous carbon by one-step carbonization of the mixture of KHCO3,urea and alginic acid.Benefiting from KHCO3 and urea syne rgistic effect,the obtained O,N-codoped hierarchical porous carbon(NPC-700) material has a well-developed interconnected porous framework with ultrahigh specific surface area(2846 m2/g) and massive heteroatoms functional groups.Consequence,such porous carbon displays high specific capacitance(324 F/g at 1 A/g),excellent rate performance(212 F/g at 30 A/g) and good electrochemical stabilization in 6 mol/L KOH solution.More importantly,the assembled NPC-700//NPC-700 symmetrical supercapacitor can achieve a high energy density of 18.8 Wh/kg and good electrochemical stabilization in 1 mol/L Na2SO4 solution.This process opens up a new way to design heteroatoms-doped hierarchical porous carbon derived from biomass materials for supercapacitors.展开更多
The hierarchical porous N/O co-functionalized carbon(HPNOC)was scalably prepared by using the lowcost and renewable blighted grains as the raw material coupled with mild KHCO_3 activation for electrochemical capacitor...The hierarchical porous N/O co-functionalized carbon(HPNOC)was scalably prepared by using the lowcost and renewable blighted grains as the raw material coupled with mild KHCO_3 activation for electrochemical capacitors(ECs).The elemental N was in situ doped in the obtained HPNOC without any N-containing additives.Remarkably,the obtained HPNOC was endowed with a large specific surface area(about 2 624m^2·g^(-1)),high pore volume(about 1.35cm^3·g^(-1)),as well as high-content N/O functionalization(about 1.9%(in atom)N and about 10.2%(in atom)O.Furthermore,the as-resulted HPNOC electrode with a high mass loading of 5mg·cm^(-2 )exhibited competitive gravimetric capacitances of about 373.6F·g^(-1 )at 0.5A·g^(-1),and even about 260.4F·g^(-1 )at a high rate of 10A·g^(-1);superior capacitance retention of about 98.8%at 1A·g^(-1 )over 10 000consecutive cycles;and high specific energy of about 9.6W·h·kg^(-1 )at a power of 500W·kg^(-1),when evaluated as a promising electrode in 6mol KOH for advanced electrochemical supercapacitors.More encouragingly,the green synthetic strategy we developed holds a huge promise in generalizing for other biomass-derived carbon materials for versatile energy-related applications.展开更多
It is a big challenge to well control the porous structure of carbon materials for supercapacitor application.Herein,a simple in-situ self-templating strategy is developed to prepare three-dimensional(3D)hierarchical ...It is a big challenge to well control the porous structure of carbon materials for supercapacitor application.Herein,a simple in-situ self-templating strategy is developed to prepare three-dimensional(3D)hierarchical porous carbons with good combination of micro and meso-porous architecture derived from a new oxygen-bridged porous organic polymer(OPOP).The OPOP is produced by the condensation polymerization of cyanuric chloride and hydroquinone in NaOH ethanol solution and NaCl is in-situ formed as by-product that will serve as template to construct an interconnected 3D hierarchical porous architecture upon carbonization.The large interface pore architecture,and rich doping of N and O heteroatoms effectively promote the electrolyte accessibility and electronic conductivity,and provide abundant active sites for energy storage.Consequently,the supercapacitors based on the optimized OPOP-800 sample display an energy density of 8.44 and 27.28 Wh·kg^(−1)in 6.0 M KOH and 1.0 M Na2SO4 electrolytes,respectively.The capacitance retention is more than 94%after 10,000 cycles.Furthermore,density functional theory(DFT)calculations have been employed to unveil the charge storage mechanism in the OPOP-800.The results presented in this job are inspiring in finely tuning the porous structure to optimize the supercapacitive performance of carbon materials.展开更多
基金Yinyu Xiang is very grateful to the China Scholarship Council(CSC:No.201806950083)for his PhD scholarship。
文摘Lithium-sulfur(Li-S)batteries,although a promising candidate of next-generation energy storage devices,are hindered by some bottlenecks in their roadmap toward commercialization.The key challenges include solving the issues such as low utilization of active materials,poor cyclic stability,poor rate performance,and unsatisfactory Coulombic efficiency due to the inherent poor electrical and ionic conductivity of sulfur and its discharged products(e.g.,Li2S2 and Li_(2)S),dissolution and migration of polysulfide ions in the electrolyte,unstable solid electrolyte interphase and dendritic growth on an odes,and volume change in both cathodes and anodes.Owing to the high specific surface area,pore volume,low density,good chemical stability,and particularly multimodal pore sizes,hierarchical porous carbon(HPC)mate rials have received considerable attention for circumventing the above pro blems in Li-S batteries.Herein,recent progress made in the synthetic methods and deployment of HPC materials for various components including sulfur cathodes,separators and interlayers,and lithium anodes in Li-S batteries is presented and summarized.More importantly,the correlation between the structures(pore volume,specific surface area,degree of pores,and heteroatom-doping)of HPC and the electrochemical performances of Li-S batteries is elaborated.Finally,a discussion on the challenges and future perspectives associated with HPCs for Li-S batteries is provided.
基金financially supported by the National Key R&D Program of China(Grants 2016YBF0100100,2016YFA0200200)the National Natural Science Foundation of China(Grants 51872283,21805273)+1 种基金the Liaoning Bai Qian Wan Talents Program,Natural Science Foundation of Liaoning Province,Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science(Grant 20180510038)the Liao Ning Revitalization Talents Program(Grant XLYC1807153),DICP(DICP ZZBS201708,DICP ZZBS201802,DICP I202032),DNL Cooperation Fund,CAS(DNL180310,DNL180308,DNL201912,and DNL201915),DICP&QIBEBT(Grant DICP&QIBEBT UN201702)。
文摘Lithium-selenium(Li-Se)batteries have attracted considerable attentions for next-generation energy storage systems owing to high volumetric capacity of 3265 m Ah cm^(-3) and excellent electronic conductivity(~10^(-5)S cm^(-1))of selenium.However,the shuttling effect and capacity fading prevent their wide applications.Herein we report a low-cost strategy for scalable fabrication of lignin derived hierarchical porous carbon(LHPC)as a new high-loading Se host for high-capacity and long-term cycling Li-Se batteries in carbonate electrolyte.The resulting LHPC exhibits three-dimensional(3D)hierarchically porous structure,high specific surface area of 1696 m^(2) g^(-1),and hetero-atom doping(O,S),which can effectively confine the Se particles into the micropores,and meanwhile,offer effective chemical binding sites for selenides from hetero-atoms(O,S).As a result,our Li-Se batteries based on Se@LHPC demonstrate high capacity of 450 m Ah g^(-1) at 0.5 C after 500 cycles,with a low capacity fading rate of only 0.027%.The theoretical simulation confirmed the strong affinity of selenides on the O and S sites of LHPC effectively mitigating the Se losing.Therefore,our strategy of using lignin as the low-cost precursor of hierarchically porous carbon for high-loading Se host offers new opportunities for high-capacity and long-life Li-Se batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.51774203)the Shenzhen Science and Technology Program(Nos.JCYJ20200109105801725)。
文摘Self-aggregation and sluggish transport kinetics of cathode materials would usually lead to the poor electrochemical performance for aqueous zinc-ion batteries(AZIBs).In this work,we report the construction of C@VO_(2) composite via anti-aggregation growth and hierarchical porous carbon encapsulation.Both of the morphology of composite and pore structure of carbon layer can be regulated by tuning the adding amount of glucose.When acting as cathode applied for AZIBs,the C@VO_(2)-3:3 composite can deliver a high capacity of 281 m Ah g^(-1) at 0.2 A g^(-1).Moreover,such cathode also exhibits a remarkably rate capability and cyclic stability,which can release a specific capacity of 195 m Ah g^(-1) at 5 A g^(-1) with the capacity retention of 95.4%after 1000 cycles.Besides that,the evolution including the crystal structure,valence state and transport kinetics upon cycling were also deeply investigated.In conclusion,benefited from the synergistic effect of anti-aggregation morphology and hierarchical porous carbon encapsulation,the building of such C@VO_(2) composite can be highly expected to enhance the ion accessible site,boost the transport kinetics and thus performing a superior storage performance.Such design concept can be applied for other kinds of electrode materials and accelerating the development of highperformance AZIBs.
基金Natural Science Foundation of Jiangsu Province,Grant/Award Number:BK20170036National Natural Science Foundation of China,Grant/Award Numbers:51572129,51772154,51811530100+1 种基金the Materials Characterization Facility of Nanjing University of Science and Technology for XRD,SEM,and TEM experiments.This study was supported by National Natural Science Foundation of China(Nos.51572129,51772154,and 51811530100)Natural Science Foundation of Jiangsu Province(No.BK20170036).
文摘Room temperature sodium-sulfur(RT Na-S)batteries are gaining extensive attention as attractive alternatives for large-scale energy storage,due to low cost and high abundancy of sodium and sulfur in nature.However,the dilemmas regarding soluble polysulfides(Na_(2)Sn,4<n<8)and the inferior reaction kinetics limit their practical application.To address these issues,we report the activated porous carbon fibers(APCF)with small sulfur molecules(S2-4)confined in ultramicropores,to achieve a reversible single-step reaction in RT Na-S batteries.The mechanism is investigated by the in situ UV/vis spectroscopy,which demonstrates Na2S is the only product during the whole discharge process.Moreover,the hierarchical carbon structure can enhance areal sulfur loading without sacrificing the capacity due to thorough contact between electrolyte and sulfur electrode.As a consequence,the APCF electrode with 38 wt%sulfur(APCF-38S)delivers a high initial reversible specific capacity of 1412 mAh g^(-1) and 10.6mAh cm^(-2)(avg.areal sulfur loading:7.5 mg cm^(-2))at 0.1 C(1C=1675 mA g^(-1)),revealing high degree of sulfur utilization.This study provides a new strategy for the development of high areal capacity RT Na-S batteries.
基金Funded by the National Program on Key Research Project of China(No.2016YFC1402406)。
文摘Hierarchical porous carbon material(MMC)was successfully fabricated via hard template synthesis method by carbonization of furfury alcohol within the template(MCM-41).The prepared MMC was studied with characterization methods including scanning electron microscopy(SEM),transmission electron microscopy(TEM),nitrogen adsorption-desorption analyses,and infrared spectral analysis(FTIR).To investigate kinetics of toluene adsorption of hierarchical porous carbon materials,the adsorption performances of these carbon samples with varying pore structure(MC-1,MMC,MMHPC)were analyzed via dynamic adsorption.And the Langmuir model and Freundlich equation were employed to correspond with adsorption isotherms to study the adsorption mechanism.The experimental results demonstrate that the Langmuir model is more appropriate to describe the adsorption process.The capacities of toluene adsorption follow the order of MMC<MMHPC(micro-meso hierarchical porous carbon)<MC-1(microporous carbon).MC-1 has satisfactory absorption performance due to its large pore volume and high ratio of micropores.MMHPC has excellent toluene adsorption performance for proper amounts of surface oxygen containing groups.Long saturation time,interconnected hierarchical pore channels,and large specific surface area make MMC also a promising material for VOCs treatment.These data reveal that the pore channel structure,rational pore distribution,high surface area and reasonable amounts of surface oxygen groups are the main factors contributed to excellent toluene adsorption performance,which proposes theoretical basis for hierarchical porous carbon materials to further engineering application.
基金supported by the Fundamental Research Funds of Shandong University(No.2016JC033)the Taishan Scholar Project of Shandong Province (No. ts201511004)
文摘Fossil fuel exhaustion and overdevelopment usually lead to a recession,which is worsened by the environmental pollution.So it is of high priority to develop high-efficiency energy storage device.Here,agreen and environment-friendly strategy is devised to fabricate carbon materials from biomass.By water extraction and alcohol precipitation,polysaccharide is extracted from loquat leaves.After calcining under high temperature,hierarchical porous carbon materials(HPCM)are obtained,possessing a variety of macropores,mesopores and micropores.Such ample and hierarchical pores enable the electrolyte infiltration and the buffering of the volume expansion of sulfur in repeated electrochemical reactions.The structure stability of the entire electrode can thus be well maintained.When evaluated as the scaffold for sulfur,the electrochemical performance of carbon/sulfur composite was tested.Even after 500 cycles,the reversible capacity is retained as high as 485.4 mA·h/g at the current density of 1.6 A/g.It also offers a notable rate capability,attaining the discharge capacity of 700.7 mA·h/g at 2 C.All the electrochemical performance results prove the feasibility of the proposed strategy.
基金the National Natural Science Foundation of China(Nos.52102036 and52301192)the Sichuan Science and Technology Program,China(No.2021JDRC0099)+3 种基金Taishan Scholars and Young Experts Program of Shandong Province,China(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution,China(Research and Innovation Team of Structural-Functional Polymer Composites)Special Financial of Shandong Province,China(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams)“Sanqin Scholars”Innovation Teams Project of Shaanxi Province,China(Clean Energy Materials and High-Performance Devices Innovation Team of Shaanxi Dongling Smelting Co.,Ltd.)。
文摘Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.
基金We acknowledge support under the Australian Research Council’s Future Fellowship(No.FT190100658,Z.H.)support from the Alexander von Humboldt Foundation(Z.H.).X.W.also acknowledges the Chinese Scholarship Council(CSC)for financial support.
文摘Dual heteroatom-doped carbons have attracted widespread research attention as catalysts in the field of energy storage and conversion due to their unique electronic structures and chemical tunability.In particular,boron and nitrogen co-doped carbon(B,N@C)has shown great potential for photo/electrocatalytic applications.However,more needs to be done for rational designing and regulating the structure of these materials to improve their catalytic performance.Herein,monodispersed hierarchical porous B,N@C nanocages were fabricated by pyrolyzing zeolite imidazole framework(ZIF)which was treated with ammonia borane or boric acid via an integrated double-solvent impregnation and nanocofined-etching method.The treated ZIF-8 provided an essential structural template to achieve B,N co-doped hierarchical structures with micro/meso/macro multimodal pore size distributions.The resultant B,N@C nanocages displayed high catalytic activities for electrochemical oxygen reduction reaction(ORR)in alkaline media,outperforming most carbon-based catalysts,particularly from the perspective of the half-wave potentials.Such high catalytic performance is due to the enhanced activity by the coexistence of B and N and the mass transfer promoted by the unique hierarchical porous structure.
基金supported by the National Key Research and Development Program of China (No.2019YFC1805804)。
文摘In this work,hydrothermal technique combined with KOH activation were employed to develop a series of porous carbons (NPCK-x) using tobacco stem as a low-cost carbon source and (NH_(4))_(2)C_(2)O_(4)as a novel nitrogen-doping agent.Physicochemical properties of NPCK-x were characterized by Brunauer-Emmett-Teller,field emission scanning electron microscopy,X-ray diffraction,Raman microscope,elemental analysis,and X-ray photoelectron spectroscopy.Results showed that the NPCK-x samples possessed large surface areas (maximum:2875 m^(2)/g),hierarchical porous structures,and high degree of disorder.N-containing functional groups decomposed during activation process,which could be the dominant reason for appearance of abundant mesopores and well-developed pore structure.Dynamic chlorobenzene adsorption experiments demonstrated that carbon materials with(NH_(4))_(2)C_(2)O_(4)modification exhibited higher adsorption capacity (maximum:1053 mg/g) than those without modification (maximum:723 mg/g).The reusability studies of chlorobenzene indicated that the desorption efficiency of (NH_(4))_(2)C_(2)O_(4)modified porous carbon reached90.40%after thermal desorption at 100℃ under N2atmosphere.Thomas model fitting results exhibited that the existence of mesopores accelerated the diffusion rate of chlorobenzene in porous carbon.Moreover,Grand Canonical Monte Carlo simulation was conducted to verify that micropores with pore sizes of 1.2–2 nm of the optimized porous carbon were the best adsorption sites for chlorobenzene and mesopores with pore sizes of 2–5 nm were also highly active sites for chlorobenzene adsorption.
基金supported financially by the National Natural Science Foundation of China (No. 21905271)Liaoning Natural Science Foundation (No. 20180510029)the Dalian National Laboratory for Clean Energy (DNL), DNL Cooperation Fund, Chinese Academy of Sciences (No. DNL180402)。
文摘The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts.
基金Projects (51272221,51072173,21203161) supported by the National Natural Science Foundation of ChinaProject (10CY005) supported by Industrial Project of Colleges and Universities of Hunan Province,China
文摘The hierarchically porous carbons (HPCs) were prepared by sol-gel selassembly technology in different surfactant concentrations and were used as the potential electrode for lithium oxygen batteries. The physical and electrochemical properties of the as-prepared HPCs were investigated by filed emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), nitrogen adsorption-desorption isotherm and galvanostatic charge/discharge. The results indicate that all of the HPCs mainly possess mesoporous structure with nearly similar pore size distribution. Using the HPCs as the electrode, a high discharge capacity for lithium oxygen battery can be achieved, and the discharge capacity increases with the specific surface area. Especially, the HPCs-3 oxygen electrode with CTAB concentration of 0.27 mol/L exhibits good capacity retention through controlling discharge depth to 800 mA·h/g and the highest discharge capacity of 2050 mA·h/g at a rate of 0.1 mA/cm2.
基金The work was financially supported by the National Natural Science of Foundation of China(No.51672114)the Natural Science Foundation of Jiangsu Province(No.BK20181469)the Zhenjiang Key Research and Development Project(Social Development)(No.SSH20190140049).
文摘Sodium-ion batteries (SIBs) have been attracting considerable attention as a promising candidate for large-scale energy storage because of the abundance and low-cost of sodium resources. However, lack of appropriate anode materials impedes further applications. Herein, a novel self-template strategy is designed to synthesize uniform flowerlike N-doped hierarchical porous carbon networks (NHPCN) with high content of N (15.31 at.%) assembled by ultrathin nanosheets via a self-synthesized single precursor and subsequent thermal annealing. Relying on the synergetic coordination of benzimidazole and 2-methylimidazole with metal ions to produce a flowerlike network, a self-formed single precursor can be harvested. Due to the structural and compositional advantages, including the high N doping, the expanded interlayer spacing, the ultrathin two-dimensional nano-sized subunits, and the three-dimensional porous network structure, these unique NHPCN flowers deliver ultrahigh reversible capacities of 453.7 mAh·g^−1 at 0.1 A·g^−1 and 242.5 mAh·g^−1 at 1 A·g^−1 for 2,500 cycles with exceptional rate capability of 5 A·g^−1 with reversible capacities of 201.2 mAh·g^−1. The greatly improved sodium storage performance of NHPCN confirms the importance of reasonable engineering and synthesis of hierarchical carbon with unique structures.
基金supported by National Program on Key Basic Research Project of China(973 Program,2012CB215500)National Natural Science Foundation of China(21361010)
文摘Advanced zinc-cerium redox flow battery(ZCRFB) is a large-scale energy storage system which plays a significant role in the application of new energy sources. The requirement of superior cathode with high acitivity and fast ion diffusion is a hierarchical porous structure, which was synthesized in this work by a method in which both hard template and soft template were used. The structure and the performance of the cathode prepared here were characterized and evaluated by a variety of techniques such as scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray photoelectron spectroscopy(XPS), cyclic voltammetry(CV), linear sweep voltammetry(LSV), and chronoamperometry(CA). There were mainly three types of pore size within the hierarchical porous carbon: 2 μm, 80 nm, and 10 nm. The charge capacity of the cell using hierarchical porous carbon(HPC) as positive electrode was obviously larger than that using carbon felt; the former was 665.5 mAh with a coulombic efficiency of 89.0% and an energy efficiency of 79.0%, whereas the latter was 611.1 mAh with a coulombic efficiency of 81.5% and an energy efficiency of 68.6%. In addition, performance of the ZCRFB using HPC as positive electrode showed a good stability over 50 cycles.These results showed that the hierarchical porous carbon was superior over the carbon felt for application in ZCRFB.
基金The work was supported by the National Natural Science Foundation of China(Nos.U2004172,51972287 and 51502269)Natural Science Foundation of Henan Province(No.202300410368)the Foundation for University Key Teacher of Henan Province(No.2020GGJS009).
文摘Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth process of lithium sulfide leads to a thick insulating film covering the electrode, inducing slow electrons transfer and mass-transfer of ions and liquid sulfur species in working Li-S cells. Here, we demonstrate a bio-inspired strategy of constructing ant-nest-like hierarchical porous ultrathin carbon nanosheet networks with the implants of metallic nanoparticles electrocatalysts (HPC-MEC) as efficient nanoreactors enabling rapid mass transfer, via a simple and green NaCl template. Such nanoreactors with a large active surface area could effectively anchor polysulfides for mitigating the shuttle effect, facilitating uniformly thin Li2S film, and promoting the mass transfer for fast sulfur species conversions. This helps contribute to a continuously high sulfur utilization in Li-S batteries with the HPC-MEC reactors. As a typical exhibition, cobalt embedded hierarchical porous carbon (HPC-Co) could realize to deliver a remarkably high specific capacity of 1,540.6 mAh·g−1, an excellent rate performance of 878.8 mAh·g−1 at 2 C, and high area capacity of 11.6 mAh·cm−2 at a high sulfur load of 10 mg·cm−2 and low electrolyte/sulfur ratio of 5 µL·mg−1.
基金supported by the National Natural Science Foundation of China(Nos.21207099 and 21273162)Science and Technology Commission of Shanghai Municipality,China(Nos. 11nm0501000 and 12ZR1451100)Key Subject of Shanghai Municipal Education Commission(No.J50102)
文摘A novel synthesis of hierarchical porous carbons (HPCs)with 3D open-cell structure based on nanosilica- embedded emulsion-templated polymerization was reported. An oil-in-water emulsion containing SiO2 colloids was fabricated using liquid paraffin as an oil phase, resorcinol/formaldehyde and silica sol as an aqueous phase, and Span 80/Tween 80 as emulsifiers. HPCs with macropore cores, open meso/ macropore windows, and abundant micropores were synthesized by the polymerization and carbonization of the emulsion, followed by scaffold removal and further KOH activation. A typical HPCs sample as supercapacitor electrode shows the charge/discharge capability under large loading current density (30 A/g) coupling with a reasonable electrochemical capacitance in KOH electrolyte solution.
基金Peng Wang and Xiaohuan Qi contributed equally to this study.This study was supported by the National Key Research and Development Program(Grant No.2016YFB0901600)National Natural Science Foundation of China(Grant Nos.21801247,51672295,51972326,and 21871008)the Key Research Program of Frontier Chinese Academy of Sciences(Grant No.QYZDJ-SSW-JSC013).
文摘Large surface area,high conductivity,and rich active site of carbon electrode materials are necessary characteristics for energy storage devices.However,high conductivity and high nitrogen doping of carbon electrode materials are difficult to coordinate.Here,a facile method via the carbonization of nitrogen-containing Schiff base polymer has been developed to prepare high conductivity and high nitrogen-doped hierarchical porous carbon.The organic components with a benzene ring structure in the polymer promote the formation of more sp^(2)-graphitized carbon,which is beneficial for the improvement of electrical conductivity.Nitrogen-doped hierarchical porous carbon calcined at 900℃ under the NH3 atmosphere possesses high nitrogen content of 7.48 at%,a large specific surface area of 1613.2m2/g,and high electrical conductivity of 2.7 S/cm.As electrode materials in an aqueous-based supercapacitor,nitrogen-doped hierarchical porous carbon exhibits superior specific capacitance of 385 F/g at 1 A/g as well as excellent rate performance(242 and 215 F/g at a current density of 100 and 200 A/g,respectively).In addition,the specific capacitance of electrode measured in a two-electrode system is 335 F/g at 1 A/g,and the long-term cycling stability can be achieved with more than 94%initial capacitance after 10000 cycles.The constructed symmetric supercapacitor delivers high energy density and high power density.The outstanding electrochemical performances combined with the novel and scalable synthetic approach make the nitrogen‐doped hierarchical porous carbon potential electrode material for electrochemical devices.
基金the financial support of National Natural Science Foundation of China(Nos.U1910201,21878208,21961024)Shanxi Province Science Foundation for Key Program(No.201901D111001(ZD))+1 种基金Inner Mongolia Natural Science Foundation(No.2018JQ05)Inner Mongolia Autonomous Region Science&Technology Planning Project for Applied Technology Research and Development(No.2019GG261)。
文摘Hierarchical porous carbon(HPC)from bituminous coal was designed and synthesized through pyrolysis foaming and KOH activation.The obtained HPC(NCF-KOH)were characterized by a high specific surface area(S_(BET))of 3472.41 m^(2)/g,appropriate mesopores with V_(mes)/V_(total)of 57%,and a proper amount of surface oxygen content(10.03%).This NCF-KOH exhibited a high specific capacitance of 487 F/g at 1.0 A/g and a rate capability of 400 F/g at 50 A/g based on the three-electrode configuration.As an electrode for a symmetric capacitor,a specific capacitance of 299 F/g at 0.5 A/g was exhibited,and the specific capacitance retained 96%of the initial capacity at 5 A/g after 10,000 cycles.Furthermore,under the power density of 249.6 W/kg in 6 mol/L KOH,a high energy density of 10.34 Wh/kg was obtained.The excellent charge storage capability benefited from its interconnected hierarchical pore structure with high accessible surface area and the suitable amount of oxygen-containing functional groups.Thus,an effective strategy to synthesize HPC for high-performance supercapacitors serves as a promising way of converting coal into advanced carbon materials.
基金financial support of the National Natural Science Foundation of China(Nos.51702043,51672055 and 51972342)Heilongjiang Postdoctoral Foundation(No.LBH-Z18008)。
文摘We report a convenient method to synthesize O,N-codoped hierarchical porous carbon by one-step carbonization of the mixture of KHCO3,urea and alginic acid.Benefiting from KHCO3 and urea syne rgistic effect,the obtained O,N-codoped hierarchical porous carbon(NPC-700) material has a well-developed interconnected porous framework with ultrahigh specific surface area(2846 m2/g) and massive heteroatoms functional groups.Consequence,such porous carbon displays high specific capacitance(324 F/g at 1 A/g),excellent rate performance(212 F/g at 30 A/g) and good electrochemical stabilization in 6 mol/L KOH solution.More importantly,the assembled NPC-700//NPC-700 symmetrical supercapacitor can achieve a high energy density of 18.8 Wh/kg and good electrochemical stabilization in 1 mol/L Na2SO4 solution.This process opens up a new way to design heteroatoms-doped hierarchical porous carbon derived from biomass materials for supercapacitors.
基金supported by the National Natural Science Foundations of China(Nos.51572005,51772127)
文摘The hierarchical porous N/O co-functionalized carbon(HPNOC)was scalably prepared by using the lowcost and renewable blighted grains as the raw material coupled with mild KHCO_3 activation for electrochemical capacitors(ECs).The elemental N was in situ doped in the obtained HPNOC without any N-containing additives.Remarkably,the obtained HPNOC was endowed with a large specific surface area(about 2 624m^2·g^(-1)),high pore volume(about 1.35cm^3·g^(-1)),as well as high-content N/O functionalization(about 1.9%(in atom)N and about 10.2%(in atom)O.Furthermore,the as-resulted HPNOC electrode with a high mass loading of 5mg·cm^(-2 )exhibited competitive gravimetric capacitances of about 373.6F·g^(-1 )at 0.5A·g^(-1),and even about 260.4F·g^(-1 )at a high rate of 10A·g^(-1);superior capacitance retention of about 98.8%at 1A·g^(-1 )over 10 000consecutive cycles;and high specific energy of about 9.6W·h·kg^(-1 )at a power of 500W·kg^(-1),when evaluated as a promising electrode in 6mol KOH for advanced electrochemical supercapacitors.More encouragingly,the green synthetic strategy we developed holds a huge promise in generalizing for other biomass-derived carbon materials for versatile energy-related applications.
基金the National Natural Science Foundation of China(No.21805235)China Postdoctoral Science Foundation(No.2017M610502)+2 种基金the Opening Foundation of Creative Platform of the Key Laboratory of the Education Department of Hunan Province(No.20K131)the Construct Program of the Key Discipline in Hunan Province is greatly acknowledged.H.C.and Z.G.L.thank the support from the Basic Research Project of the Science and Technology Innovation Commission of Shenzhen(No.JCYJ20170817110251498)Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials(No.ZDSYS20200421111401738).
文摘It is a big challenge to well control the porous structure of carbon materials for supercapacitor application.Herein,a simple in-situ self-templating strategy is developed to prepare three-dimensional(3D)hierarchical porous carbons with good combination of micro and meso-porous architecture derived from a new oxygen-bridged porous organic polymer(OPOP).The OPOP is produced by the condensation polymerization of cyanuric chloride and hydroquinone in NaOH ethanol solution and NaCl is in-situ formed as by-product that will serve as template to construct an interconnected 3D hierarchical porous architecture upon carbonization.The large interface pore architecture,and rich doping of N and O heteroatoms effectively promote the electrolyte accessibility and electronic conductivity,and provide abundant active sites for energy storage.Consequently,the supercapacitors based on the optimized OPOP-800 sample display an energy density of 8.44 and 27.28 Wh·kg^(−1)in 6.0 M KOH and 1.0 M Na2SO4 electrolytes,respectively.The capacitance retention is more than 94%after 10,000 cycles.Furthermore,density functional theory(DFT)calculations have been employed to unveil the charge storage mechanism in the OPOP-800.The results presented in this job are inspiring in finely tuning the porous structure to optimize the supercapacitive performance of carbon materials.