Pristine tin (Sn) and tin dioxide (SnO_(2)) have sparked wide interest owing to their abundant resources and superior theoretical capacity. Nevertheless, the obvious volume expansion effect upon cycling and undesirabl...Pristine tin (Sn) and tin dioxide (SnO_(2)) have sparked wide interest owing to their abundant resources and superior theoretical capacity. Nevertheless, the obvious volume expansion effect upon cycling and undesirable conductivity of Sn-based materials lead to undesirable specific capacity. In this work, a nanostructured Sn/SnO_(2)/nitrogen-doped carbon (NC) superstructure was prepared through a facile electrospray-carbonization strategy. The Sn/SnO_(2) nanoparticles (NPs) were uniformly dispersed in a spherical NC matrix, which prevented the volume expansion and aggregation of NPs and facilitated the ion diffusion and charge transfer kinetics. When the optimized Sn/SnO_(2)/NC superstructures were employed as lithium-ion battery anodes, a remarkable specific capacity of 747.9 mAh·g^(−1) over 200 cycles at 0.5 A·g^(−1) and a superior cyclability of 644.1 mAh·g^(−1) over 1000 cycles at 2 A·g^(−1) were obtained. This effective synthetic strategy for synthesizing superstructures provides valuable insights for the advancement of lithium-ion batteries.展开更多
Carbon quantum dots (CQDs) have been used in memristors due to their attractive optical and electronic properties, which are considered candidates for brain-inspired computing devices. In this work, the performance of...Carbon quantum dots (CQDs) have been used in memristors due to their attractive optical and electronic properties, which are considered candidates for brain-inspired computing devices. In this work, the performance of CQDs-based memristors is improved by utilizing nitrogen-doping. In contrast, nitrogen-doped CQDs (N-CQDs)-based optoelectronic memristors can be driven with smaller programming voltages (−0.6 to 0.7 V) and exhibit lower powers (78 nW/0.29 µW). The physical mechanism can be attributed to the reversible transition between C–N and C=N with lower binding energy induced by the electric field and the generation of photogenerated carriers by ultraviolet light irradiation, which adjusts the conductivity of the initial N-CQDs to implement resistance switching. Importantly, the convolutional image processing based on various cross kernels is efficiently demonstrated by stable multi-level storage properties. An N-CQDs-based optoelectronic reservoir computing implements impressively high accuracy in both no noise and various noise modes when recognizing the Modified National Institute of Standards and Technology (MNIST) dataset. It illustrates that N-CQDs-based memristors provide a novel strategy for developing artificial vision system with integrated in-memory sensor and computing.展开更多
The problems of electromagnetic wave(EMW)pollution in X and Ku bands(8–18 GHz)are becoming more and more serious.Therefore,it is urgent to design EMW absorbing materials with high-efficiency such as thin thickness,li...The problems of electromagnetic wave(EMW)pollution in X and Ku bands(8–18 GHz)are becoming more and more serious.Therefore,it is urgent to design EMW absorbing materials with high-efficiency such as thin thickness,lightweight,wide bandwidth and strong EMW absorption.Inspired by the biomorph of sea cucumber,Nb_(2)CT_(x) MXene@Co nitrogen-doped carbon nanosheet arrays@carbon fiber aerogels(Nb_(2)CT_(x)@Co-NC@CFA,Nb_(2)CT_(x)=niobium carbide)were constructed by self-assembly,in-situ chemical deposition and subsequent pyrolysis.The carbon fiber aerogel,as the basic skeleton of sea cucumber,forms lightweight three-dimensional interconnected conductive network,enhances the dielectric loss and extends the multiple reflection and absorption paths of EMW.As the tentacles of sea cucumber surface,Nb_(2)CT_(x) MXene and Co nitrogen-doped carbon nanosheet arrays exist rich heterogeneous interfaces,which play an important role in improving EMW polarization loss and optimizing impedance matching.The minimum reflection loss(RLmin)of Nb_(2)CT_(x)@Co-NC@CFA reaches−54.7 dB at 9.84 GHz(2.36 mm)with a low filling ratio of 10 wt.%and the effective absorption bandwidth(EAB)of Nb_(2)CT_(x)@Co-NC@CFA reaches 2.96 GHz(8.48–11.44 GHz)with 2.36 mm and 5.2 GHz(12.8–18 GHz)with 1.6 mm,covering most of X and Ku bands by adjusting thickness.The radar cross section(RCS)value of Nb_(2)CT_(x)@Co-NC@CFA is 26.64 dB·m^(2),which is lower than that of the perfect electrical conductor(PEC),indicating that Nb_(2)CT_(x)@Co-NC@CFA can effectively decrease the probability of the target being detected by the radar detector.This work provides ideas for design and development of EMW absorbing materials with high-efficiency EMW absorption in X and Ku bands.展开更多
Carbon nanofiber(CNF)was widely utilized in the field of electrochemical energy storage due to its superiority of conductivity and mechanics.However,CNF was generally prepared at relatively high temperature.Herein,nit...Carbon nanofiber(CNF)was widely utilized in the field of electrochemical energy storage due to its superiority of conductivity and mechanics.However,CNF was generally prepared at relatively high temperature.Herein,nitrogen-doped hard carbon nanofibers(NHCNFs)were prepared by a lowtemperature carbonization treatment assisted with electrospinning technology.Density functional theory analysis elucidates the incorporation of nitrogen heteroatoms with various chemical states into carbon matrix would significantly alter the total electronic configurations,leading to the robust adsorption and efficient diffusion of Na atoms on electrode interface.The obtained material carbonized at 600°C(NHCNF-600)presented a reversible specific capacity of 191.0 mAh g^(−1)and no capacity decay after 200 cycles at 1 A g^(−1).It was found that the sodium-intercalated degree had a correlation with the electrochemical impedance.A sodium-intercalated potential of 0.2 V was adopted to lower the electrochemical impedance.The constructed sodium-ion capacitor with activated carbon cathode and presodiated NHCNF-600 anode can present an energy power density of 82.1 Wh kg^(−1)and a power density of 7.0 kW kg^(−1).展开更多
The oxygen reduction reaction(ORR)electrocatalytic activity of Pt-based catalysts can be significantly improved by supporting Pt and its alloy nanoparticles(NPs)on a porous carbon support with large surface area.Howev...The oxygen reduction reaction(ORR)electrocatalytic activity of Pt-based catalysts can be significantly improved by supporting Pt and its alloy nanoparticles(NPs)on a porous carbon support with large surface area.However,such catalysts are often obtained by constructing porous carbon support followed by depositing Pt and its alloy NPs inside the pores,in which the migration and agglomeration of Pt NPs are inevitable under harsh operating conditions owing to the relatively weak interaction between NPs and carbon support.Here we develop a facile electrospinning strategy to in-situ prepare small-sized PtZn NPs supported on porous nitrogen-doped carbon nanofibers.Electrochemical results demonstrate that the as-prepared PtZn alloy catalyst exhibits excellent initial ORR activity with a half-wave potential(E_(1/2))of 0.911 V versus reversible hydrogen electrode(vs.RHE)and enhanced durability with only decreasing 11 mV after 30,000 potential cycles,compared to a more significant drop of 24 mV in E_(1/2)of Pt/C catalysts(after 10,000 potential cycling).Such a desirable performance is ascribed to the created triple-phase reaction boundary assisted by the evaporation of Zn and strengthened interaction between nanoparticles and the carbon support,inhibiting the migration and aggregation of NPs during the ORR.展开更多
Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged inter...Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous structures.The structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron microscopy.Due to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 cycles.This research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.展开更多
Hierarchical nitrogen-doped carbon nanocages (hNCNC) with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with...Hierarchical nitrogen-doped carbon nanocages (hNCNC) with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with 20 wt% loading has a homogeneous dispersion of Pt nanoparticles with the average size of 3.3 nm, which is smaller than 4.3 and 4.9 nm for the control catalysts with the same loading supported on hierarchical carbon nanocages (hCNC) and commercial Vulcan XC-72, respec- tively. Accordingly, Pt/hNCNC has a larger electrochemical surface area than Pt/hCNC and Pt/XC-72. The Pt/hNCNC catalyst exhibited excellent electrocatalytic activity and stability for methanol oxidation, which was better than the control catalysts. This was attributed to the en- hanced interaction between Pt and hNCNC due to nitrogen participation in the anchoring function. By making use of the unique advantages of the hNCNC support, a heavy Pt loading up to 60 wt% was prepared without serious agglomeration, which gave a high peak-current density per unit mass of catalyst of 95.6 mA/mg for achieving a high power density. These results showed the potential of the Pt/hNCNC catalyst for methanol oxidation and of the new hNCNC support for wide applications.展开更多
The oxygen reduction reaction (ORR) is traditionally performed using noble‐metals catalysts, e.g. Pt. However, these metal‐based catalysts have the drawbacks of high costs, low selectivity, poor stabili‐ties, and...The oxygen reduction reaction (ORR) is traditionally performed using noble‐metals catalysts, e.g. Pt. However, these metal‐based catalysts have the drawbacks of high costs, low selectivity, poor stabili‐ties, and detrimental environmental effects. Here, we describe metal‐free nitrogen‐doped carbon nanoblocks (NCNBs) with high nitrogen contents (4.11%), which have good electrocatalytic proper‐ties for ORRs. This material was fabricated using a scalable, one‐step process involving the pyrolysis of tris(hydroxymethyl)aminomethane (Tris) at 800℃. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is-0.05 V (vs Ag/AgCl), the ORR reduction peak potential is-0.20 V (vs Ag/AgCl), and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long‐term stability, and better tolerance of the methanol crosso‐ver effect compared with a commercial 20 wt%Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier‐transform infrared spectroscopy, scanning electron microscopy, X‐ray photoelectron spectroscopy, and X‐ray diffraction. The pyroly‐sis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.展开更多
Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air...Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air batteries. Herein, an efficient bifunctional electrocatalyst based on hollow cobalt oxide nanoparticles embedded in nitrogen-doped carbon nanosheets(Co/N-Pg) is fabricated for Zn–air batteries. A lowcost biomass peach gum, consisting of carbon, oxygen, and hydrogen without other heteroatoms, was used as carbon source to form carbon matrix hosting hollow cobalt oxide nanoparticles. Meanwhile, the melamine was applied as nitrogen source and template precursor, which can convert to carbon-based template graphitic carbon nitride by polycondensation process. Owing to the unique structure and synergistic effect between hollow cobalt oxide nanoparticles and Co-N-C species, the proposal Co/N-Pg catalyst displays not only prominent bifunctional electrocatalytic activities for ORR and OER, but also excellent durability. Remarkably, the assembled Zn–air battery with Co/N-Pg air electrode exhibited a low discharge-charge voltage gap(0.81 V at 50 mA cm^-2) and high peak power density(119 mW cm^-2) with long-term cycling stability. This work presents an effective approach for engineering transition metal oxides and nitrogen modified carbon nanosheets to boost the performance of bifunctional electrocatalysts for Zn–air battery.展开更多
Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we ...Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon (HPNC) via acombination of salt template (ZnC12) and hard template (SiO2) as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC (IC= 1675 mAh g^-1 ), a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.展开更多
Potassium-ion batteries(KIBs)have great potential for applications in large-scale energy storage devices.However,the larger radius of K+leads to sluggish kinetics and inferior cycling performance,severely restricting ...Potassium-ion batteries(KIBs)have great potential for applications in large-scale energy storage devices.However,the larger radius of K+leads to sluggish kinetics and inferior cycling performance,severely restricting its practical applicability.Herein,we propose a rational strategy involving a Prussian blue analogue-derived graphitized carbon anode with fast and durable potassium storage capability,which is constructed by encapsulating cobalt nanoparticles in nitrogen-doped graphitized carbon(Co-NC).Both experimental and theoretical results show that N-doping effectively promotes the uniform dispersion of cobalt nanoparticles in the carbon matrix through Co-N bonds.Moreover,the cobalt nanoparticles and strong Co-N bonds synergistically form a threedimensional conductive network,increase the number of adsorption sites,and reduce the diffusion energy barrier,thereby facilitating the adsorption and the diffusion kinetics.These multiple effects lead to enhanced reversible capacities of 305 and 208.6 mAh g^−1 after 100 and 300 cycles at 0.05 and 0.1 A g^−1,respectively,demonstrating the applicability of the Co-NC anode for KIBs.展开更多
Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and...Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and is therefore of great interest from an academic and industrial point of view. Very recently,novel metal-free mesoporous nitrogen-doped carbon catalysts have attracted large attention due to the unique reactivity and selectivity for the electrochemical hydrogen peroxide formation [1–3]. In this work,we provide deeper insights into the electrocatalytic activity, selectivity and durability of novel metal-free mesoporous nitrogen-doped carbon catalyst for the peroxide formation with a particular emphasis on the influence of experimental reaction parameters such as p H value and electrode potential for three different electrolytes. We used two independent approaches for the investigation of electrochemical hydrogen peroxide formation, namely rotating ring-disk electrode(RRDE) technique and photometric UV–VIS technique. Our electrochemical and photometric results clearly revealed a considerable peroxide formation activity as well as high catalyst durability for the metal-free nitrogen-doped carbon catalyst material in both acidic as well as neutral medium at the same electrode potential under ambient temperature and pressure. In addition, the obtained electrochemical reactivity and selectivity indicate that the mechanisms for the electrochemical formation and decomposition of peroxide are strongly dependent on the p H value and electrode potential.展开更多
High-value reclamation of metal-polluted plants involved in phytoremediation is a big challenge.In this study,nitrogen-doped nanoporous carbon with large specific area of 2359.1 m^(2)g^(-1) is facilely fabricated from...High-value reclamation of metal-polluted plants involved in phytoremediation is a big challenge.In this study,nitrogen-doped nanoporous carbon with large specific area of 2359.1 m^(2)g^(-1) is facilely fabricated from metal-polluted miscanthus waste for efficient energy storage.The synergistic effect of KOH,urea and ammonia solution greatly improve the nitrogen quantity and surface area of the synthesized carbon.Electrodes fabricated with this carbon exhibit the excellent capacitance performance of 340.2 F g^(-1) at 0.5 A g^(-1) and a low combined resistance of 0.116Ω,which are competitive with most of previously reported carbon-based electrodes.In addition,the as-obtained carbon electrode shows a high specific capacitance retention of over 99.6%even after 5000 cycles.Furthermore,the symmetric supercapacitor fabricated using the synthesized carbon achieves a superior energy density of 25.3 Wh kg^(-1)(at 400 W kg^(-1))in 1 mol L^(-1) Na_(2)SO_(4)aqueous solution.This work provides an efficient route to upcycle metal-polluted plant waste for supercapacitor applications.展开更多
Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons(NOMCs) by the nanocasting method.The effect of the ...Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons(NOMCs) by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy(XPS),cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole(C-PY-900:765 m^2/) and phenanthroline(C-Phen-900:746 m^2/) exhibit higher specific surface areas than the aniline analog(C-PA-900:569 m^2/).Second,the XPS results indicate that the total nitrogen content(ca.3.1–3.3 at%) is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction(ORR).In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.展开更多
Yellowish nitrogen-doped titania was produced through sol-gel method in mild condition, with the elemental nitrogen derived from aqua ammonia. The titania catalysts were characterized using XRD, BET, TEM, XPS, and UV-...Yellowish nitrogen-doped titania was produced through sol-gel method in mild condition, with the elemental nitrogen derived from aqua ammonia. The titania catalysts were characterized using XRD, BET, TEM, XPS, and UV-Vis diffuse reflectance spectrophotometer, and their photocatalytic activities were evaluated under UV and visible light, respec tively. The XRD results showed that all titania catalysts were anatase. More significantly, the crystallite size of nitrogen-doped titania increased with an increase in N/Ti proportion, and the doping of nitrogen could extend the absorption shoulder into the visible-light region, thus it possessed a higher visible-light activity illustrated by decolorization of methyl orange (65.3%) under the irradiation of visible light, whereas pure titania showed little of such kind of visible light activity. The UV-light activity of nitrogen-doped titania catalysts was worse than that of pure titania and Degussa P25. In the range of N/Ti proportion of 4-10 mol%, the activity of nitrogen-doped titania weakened appreciably in the visible-light region as the N/Ti proportion increased, whereas a reverse relationship existed under the irradiation of UV light.展开更多
A novel Ag@nitrogen-doped porous carbon(Ag-NPC) composite was synthesized via a facile hydrothermal method and applied as an anode material in lithium-ion batteries(LIBs). Using this method, Ag nanoparticles(Ag NPs) w...A novel Ag@nitrogen-doped porous carbon(Ag-NPC) composite was synthesized via a facile hydrothermal method and applied as an anode material in lithium-ion batteries(LIBs). Using this method, Ag nanoparticles(Ag NPs) were embedded in NPC through thermal decomposition of Ag NO_3 in the pores of NPC. The reversible capacity of Ag-NPC remained at 852 m Ah g^(-1)after 200 cycles at a current density of 0.1 A g^(-1), showing its remarkable cycling stability. The enhancement of the electrochemical properties such as cycling performance,reversible capacity and rate performance of Ag-NPC compared to the NPC contributed to the synergistic effects between Ag NPs and NPC.展开更多
Nitrogen-doped carbon nanotubes (NCNTs) were used as a support for iron (Fe) nanoparticles applied in car- bon dioxide (CO_2) hydrogenation at 633 K and 25 bar (1 bar = 10-5 Pa). The Fe/NCNT catalyst promoted ...Nitrogen-doped carbon nanotubes (NCNTs) were used as a support for iron (Fe) nanoparticles applied in car- bon dioxide (CO_2) hydrogenation at 633 K and 25 bar (1 bar = 10-5 Pa). The Fe/NCNT catalyst promoted with both potassium (K) and manganese (Mn) showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity (GHSV) of 3.1 L-(g·h)-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction (XRD), temperature-programmed reduction (TPR) with molecular hydrogen (H2), and in situ X-ray absorption near-edge structure (XANES) analysis. The Mn pro- moter stabilized wtistite (FeO) as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia (NH_3) decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.展开更多
Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt s...Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube(N–CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N–CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc–air battery.展开更多
In this paper, nitrogen-doped hierarchical porous carbon(N-HPC) was prepared from polyaniline(PANI)/silica self-aggregates. H-bonding between N\\H groups in aniline/PANI and \\OH groups in nano silica template led to ...In this paper, nitrogen-doped hierarchical porous carbon(N-HPC) was prepared from polyaniline(PANI)/silica self-aggregates. H-bonding between N\\H groups in aniline/PANI and \\OH groups in nano silica template led to a self-assembly type, which enabled the formation of uniform N-HPC nanoparticles. Silica self-aggregates provided macroporous channels resulted in a decreased diffusion distance. After removing the hard template,the N-HPC had a high surface area(899 m^2·g^(-1)). Owing to two co-existed synergetic energy-storage mechanisms and the hierarchical porous structure, the obtained N-HPC exhibited a high specific capacitance of 218.75 F·g^(-1) at 0.5 A·g^(-1), compared with the nonporous nitrogen-doped carbon(N-C) derived from pure PANI. Moreover, the N-HPC electrode demonstrated excellent cycle life, retaining 99% of its initial specific capacitance after 1000 cycles.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
基金supported by the National Natural Science Foundation of China(No.52371240)Natural Science Foundation of Jiangsu Province(No.BK20230556)+1 种基金China Postdoctoral Science Foundation(No.2022M722686)Jiangsu Funding Program for Excellent Postdoctoral Talent(No.2023ZB701).
文摘Pristine tin (Sn) and tin dioxide (SnO_(2)) have sparked wide interest owing to their abundant resources and superior theoretical capacity. Nevertheless, the obvious volume expansion effect upon cycling and undesirable conductivity of Sn-based materials lead to undesirable specific capacity. In this work, a nanostructured Sn/SnO_(2)/nitrogen-doped carbon (NC) superstructure was prepared through a facile electrospray-carbonization strategy. The Sn/SnO_(2) nanoparticles (NPs) were uniformly dispersed in a spherical NC matrix, which prevented the volume expansion and aggregation of NPs and facilitated the ion diffusion and charge transfer kinetics. When the optimized Sn/SnO_(2)/NC superstructures were employed as lithium-ion battery anodes, a remarkable specific capacity of 747.9 mAh·g^(−1) over 200 cycles at 0.5 A·g^(−1) and a superior cyclability of 644.1 mAh·g^(−1) over 1000 cycles at 2 A·g^(−1) were obtained. This effective synthetic strategy for synthesizing superstructures provides valuable insights for the advancement of lithium-ion batteries.
基金financially supported by the National Key Research and Development Program of China(No.2022YFE0139100)International cooperative research project of Jiangsu province(No.BZ2022008)+3 种基金the National Natural Science Foundation Project of China(No.62175028)Program 111_2.0 in China(No.BP0719013)Leading Technology of Jiangsu Basic Research Plan(No.BK20192003)Postgraduate Research & Practice Innovation Program of Jiangsu Province,the Fundamental Research Funds for the Central Universities(No.KYCX23_0254).
文摘Carbon quantum dots (CQDs) have been used in memristors due to their attractive optical and electronic properties, which are considered candidates for brain-inspired computing devices. In this work, the performance of CQDs-based memristors is improved by utilizing nitrogen-doping. In contrast, nitrogen-doped CQDs (N-CQDs)-based optoelectronic memristors can be driven with smaller programming voltages (−0.6 to 0.7 V) and exhibit lower powers (78 nW/0.29 µW). The physical mechanism can be attributed to the reversible transition between C–N and C=N with lower binding energy induced by the electric field and the generation of photogenerated carriers by ultraviolet light irradiation, which adjusts the conductivity of the initial N-CQDs to implement resistance switching. Importantly, the convolutional image processing based on various cross kernels is efficiently demonstrated by stable multi-level storage properties. An N-CQDs-based optoelectronic reservoir computing implements impressively high accuracy in both no noise and various noise modes when recognizing the Modified National Institute of Standards and Technology (MNIST) dataset. It illustrates that N-CQDs-based memristors provide a novel strategy for developing artificial vision system with integrated in-memory sensor and computing.
基金financially supported by the National Natural Science Foundation of China and the Civil Aviation Administration of China(No.U1833118)the Open Project Program of High-Tech Organic Fibers Key Laboratory of Sichuan Province(No.PLN2022-10)+3 种基金the Science and Technology Plan Project of Chengdu City(2022-YF05-00411-SN)Science and Technology Planning Project of Sichuan Province(Nos.2023YFQ0090,2024YFHZ0218,2023YFN0016,and 2023YFQ083)Yibin Science and Technology Plan Project(No.2022JB013)Engineering characteristic team of Sichuan University(No.2020SCUNG122).
文摘The problems of electromagnetic wave(EMW)pollution in X and Ku bands(8–18 GHz)are becoming more and more serious.Therefore,it is urgent to design EMW absorbing materials with high-efficiency such as thin thickness,lightweight,wide bandwidth and strong EMW absorption.Inspired by the biomorph of sea cucumber,Nb_(2)CT_(x) MXene@Co nitrogen-doped carbon nanosheet arrays@carbon fiber aerogels(Nb_(2)CT_(x)@Co-NC@CFA,Nb_(2)CT_(x)=niobium carbide)were constructed by self-assembly,in-situ chemical deposition and subsequent pyrolysis.The carbon fiber aerogel,as the basic skeleton of sea cucumber,forms lightweight three-dimensional interconnected conductive network,enhances the dielectric loss and extends the multiple reflection and absorption paths of EMW.As the tentacles of sea cucumber surface,Nb_(2)CT_(x) MXene and Co nitrogen-doped carbon nanosheet arrays exist rich heterogeneous interfaces,which play an important role in improving EMW polarization loss and optimizing impedance matching.The minimum reflection loss(RLmin)of Nb_(2)CT_(x)@Co-NC@CFA reaches−54.7 dB at 9.84 GHz(2.36 mm)with a low filling ratio of 10 wt.%and the effective absorption bandwidth(EAB)of Nb_(2)CT_(x)@Co-NC@CFA reaches 2.96 GHz(8.48–11.44 GHz)with 2.36 mm and 5.2 GHz(12.8–18 GHz)with 1.6 mm,covering most of X and Ku bands by adjusting thickness.The radar cross section(RCS)value of Nb_(2)CT_(x)@Co-NC@CFA is 26.64 dB·m^(2),which is lower than that of the perfect electrical conductor(PEC),indicating that Nb_(2)CT_(x)@Co-NC@CFA can effectively decrease the probability of the target being detected by the radar detector.This work provides ideas for design and development of EMW absorbing materials with high-efficiency EMW absorption in X and Ku bands.
基金supported by the National Natural Science Foundation of China(No.51907193,51822706,and 51777200)the Key Research Program of Frontier Sciences,CAS(No.ZDBS-LY-JSC047)the Youth Innovation Promotion Association,CAS(No.2020145)
文摘Carbon nanofiber(CNF)was widely utilized in the field of electrochemical energy storage due to its superiority of conductivity and mechanics.However,CNF was generally prepared at relatively high temperature.Herein,nitrogen-doped hard carbon nanofibers(NHCNFs)were prepared by a lowtemperature carbonization treatment assisted with electrospinning technology.Density functional theory analysis elucidates the incorporation of nitrogen heteroatoms with various chemical states into carbon matrix would significantly alter the total electronic configurations,leading to the robust adsorption and efficient diffusion of Na atoms on electrode interface.The obtained material carbonized at 600°C(NHCNF-600)presented a reversible specific capacity of 191.0 mAh g^(−1)and no capacity decay after 200 cycles at 1 A g^(−1).It was found that the sodium-intercalated degree had a correlation with the electrochemical impedance.A sodium-intercalated potential of 0.2 V was adopted to lower the electrochemical impedance.The constructed sodium-ion capacitor with activated carbon cathode and presodiated NHCNF-600 anode can present an energy power density of 82.1 Wh kg^(−1)and a power density of 7.0 kW kg^(−1).
基金This work was financially supported by National Key Research and Development Program(2018YFB1502503).
文摘The oxygen reduction reaction(ORR)electrocatalytic activity of Pt-based catalysts can be significantly improved by supporting Pt and its alloy nanoparticles(NPs)on a porous carbon support with large surface area.However,such catalysts are often obtained by constructing porous carbon support followed by depositing Pt and its alloy NPs inside the pores,in which the migration and agglomeration of Pt NPs are inevitable under harsh operating conditions owing to the relatively weak interaction between NPs and carbon support.Here we develop a facile electrospinning strategy to in-situ prepare small-sized PtZn NPs supported on porous nitrogen-doped carbon nanofibers.Electrochemical results demonstrate that the as-prepared PtZn alloy catalyst exhibits excellent initial ORR activity with a half-wave potential(E_(1/2))of 0.911 V versus reversible hydrogen electrode(vs.RHE)and enhanced durability with only decreasing 11 mV after 30,000 potential cycles,compared to a more significant drop of 24 mV in E_(1/2)of Pt/C catalysts(after 10,000 potential cycling).Such a desirable performance is ascribed to the created triple-phase reaction boundary assisted by the evaporation of Zn and strengthened interaction between nanoparticles and the carbon support,inhibiting the migration and aggregation of NPs during the ORR.
基金financially supported by the National Natural Science Foundation of China(Nos.21873026,21573061,21773059)。
文摘Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous structures.The structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron microscopy.Due to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 cycles.This research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.
基金supported by the National Natural Science Foundation of China(21473089,51232003,21373108,51571110,21573107)the Nation-al Basic Research Program of China(973 Program,2013CB932902)+2 种基金Suzhou Science and Technology Projects(ZXG2013025)Changzhou Science and Technology Projects(CE20130032)supported by a Project Funded by the Technology Support Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Hierarchical nitrogen-doped carbon nanocages (hNCNC) with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with 20 wt% loading has a homogeneous dispersion of Pt nanoparticles with the average size of 3.3 nm, which is smaller than 4.3 and 4.9 nm for the control catalysts with the same loading supported on hierarchical carbon nanocages (hCNC) and commercial Vulcan XC-72, respec- tively. Accordingly, Pt/hNCNC has a larger electrochemical surface area than Pt/hCNC and Pt/XC-72. The Pt/hNCNC catalyst exhibited excellent electrocatalytic activity and stability for methanol oxidation, which was better than the control catalysts. This was attributed to the en- hanced interaction between Pt and hNCNC due to nitrogen participation in the anchoring function. By making use of the unique advantages of the hNCNC support, a heavy Pt loading up to 60 wt% was prepared without serious agglomeration, which gave a high peak-current density per unit mass of catalyst of 95.6 mA/mg for achieving a high power density. These results showed the potential of the Pt/hNCNC catalyst for methanol oxidation and of the new hNCNC support for wide applications.
基金supported by the National Natural Science Foundation of China (21375088,21575090)Scientific Research Project of Beijing Educational Committee (KM201410028006)+1 种基金Scientific Research Base Development Program of the Beijing Municipal Commission of EducationYouth Talent Project of the Beijing Municipal Commission of Education (CIT & TCD201504072)~~
文摘The oxygen reduction reaction (ORR) is traditionally performed using noble‐metals catalysts, e.g. Pt. However, these metal‐based catalysts have the drawbacks of high costs, low selectivity, poor stabili‐ties, and detrimental environmental effects. Here, we describe metal‐free nitrogen‐doped carbon nanoblocks (NCNBs) with high nitrogen contents (4.11%), which have good electrocatalytic proper‐ties for ORRs. This material was fabricated using a scalable, one‐step process involving the pyrolysis of tris(hydroxymethyl)aminomethane (Tris) at 800℃. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is-0.05 V (vs Ag/AgCl), the ORR reduction peak potential is-0.20 V (vs Ag/AgCl), and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long‐term stability, and better tolerance of the methanol crosso‐ver effect compared with a commercial 20 wt%Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier‐transform infrared spectroscopy, scanning electron microscopy, X‐ray photoelectron spectroscopy, and X‐ray diffraction. The pyroly‐sis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.
基金financially supported by the National Natural Science Foundation of China (Nos. 21506081, 21705058, 21676126)the Provincial Natural Science Foundation of Jiangsu (Nos. BK20170524, BK20160492)+2 种基金China Postdoctoral Science Foundation (No. 2018T110450)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education InstitutionsThe financial support from an ARC Discovery Project (No. DP180102003)
文摘Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air batteries. Herein, an efficient bifunctional electrocatalyst based on hollow cobalt oxide nanoparticles embedded in nitrogen-doped carbon nanosheets(Co/N-Pg) is fabricated for Zn–air batteries. A lowcost biomass peach gum, consisting of carbon, oxygen, and hydrogen without other heteroatoms, was used as carbon source to form carbon matrix hosting hollow cobalt oxide nanoparticles. Meanwhile, the melamine was applied as nitrogen source and template precursor, which can convert to carbon-based template graphitic carbon nitride by polycondensation process. Owing to the unique structure and synergistic effect between hollow cobalt oxide nanoparticles and Co-N-C species, the proposal Co/N-Pg catalyst displays not only prominent bifunctional electrocatalytic activities for ORR and OER, but also excellent durability. Remarkably, the assembled Zn–air battery with Co/N-Pg air electrode exhibited a low discharge-charge voltage gap(0.81 V at 50 mA cm^-2) and high peak power density(119 mW cm^-2) with long-term cycling stability. This work presents an effective approach for engineering transition metal oxides and nitrogen modified carbon nanosheets to boost the performance of bifunctional electrocatalysts for Zn–air battery.
基金financially supported by the National Key Research and Development Program of China (2016YFB0101202)the NSFC of China (Grants 91534205,21436003 and 21576031)Graduate Research and Innovation Foundation of Chongqing China (Grant No.CYB17021)
文摘Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon (HPNC) via acombination of salt template (ZnC12) and hard template (SiO2) as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC (IC= 1675 mAh g^-1 ), a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.
基金supported by National Natural Science Foundation of China(Grant No.51932011,51802356)Innovation-Driven Project of Central South University(No.2020CX024)+3 种基金the Research Support Fund of the Collaborative Innovation Center of Manganese-Zinc-Vanadium Industrial Technology in Hunan Province(No.201809)the Program of Youth Talent Support for Hunan Province(2018RS3098)Hunan Provincial Innovation Foundation for Postgraduate(Grant No.CX2017B045)the Fundamental Research Funds for the Central Universities of Central South University(Grant No.2020zzts075).
文摘Potassium-ion batteries(KIBs)have great potential for applications in large-scale energy storage devices.However,the larger radius of K+leads to sluggish kinetics and inferior cycling performance,severely restricting its practical applicability.Herein,we propose a rational strategy involving a Prussian blue analogue-derived graphitized carbon anode with fast and durable potassium storage capability,which is constructed by encapsulating cobalt nanoparticles in nitrogen-doped graphitized carbon(Co-NC).Both experimental and theoretical results show that N-doping effectively promotes the uniform dispersion of cobalt nanoparticles in the carbon matrix through Co-N bonds.Moreover,the cobalt nanoparticles and strong Co-N bonds synergistically form a threedimensional conductive network,increase the number of adsorption sites,and reduce the diffusion energy barrier,thereby facilitating the adsorption and the diffusion kinetics.These multiple effects lead to enhanced reversible capacities of 305 and 208.6 mAh g^−1 after 100 and 300 cycles at 0.05 and 0.1 A g^−1,respectively,demonstrating the applicability of the Co-NC anode for KIBs.
基金supported by the Technische Universitat Berlin,the Max Planck Society and the Cluster of Excellence“Unifying Concepts in Catalysis(Uni Cat)”
文摘Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and is therefore of great interest from an academic and industrial point of view. Very recently,novel metal-free mesoporous nitrogen-doped carbon catalysts have attracted large attention due to the unique reactivity and selectivity for the electrochemical hydrogen peroxide formation [1–3]. In this work,we provide deeper insights into the electrocatalytic activity, selectivity and durability of novel metal-free mesoporous nitrogen-doped carbon catalyst for the peroxide formation with a particular emphasis on the influence of experimental reaction parameters such as p H value and electrode potential for three different electrolytes. We used two independent approaches for the investigation of electrochemical hydrogen peroxide formation, namely rotating ring-disk electrode(RRDE) technique and photometric UV–VIS technique. Our electrochemical and photometric results clearly revealed a considerable peroxide formation activity as well as high catalyst durability for the metal-free nitrogen-doped carbon catalyst material in both acidic as well as neutral medium at the same electrode potential under ambient temperature and pressure. In addition, the obtained electrochemical reactivity and selectivity indicate that the mechanisms for the electrochemical formation and decomposition of peroxide are strongly dependent on the p H value and electrode potential.
基金financial supports from KeyArea Research and Development Program of Guangdong Province(2019B110209003)Guangdong Basic and Applied Basic Research Foundation(2019B1515120058,2020A1515011149)+3 种基金National Key R&D Program of China(2018YFD0800700)National Ten Thousand Talent Plan,National Natural Science Foundation of China(21776324)the Fundamental Research Funds for the Central Universities(19lgzd25)Hundred Talent Plan(201602)from Sun Yatsen University。
文摘High-value reclamation of metal-polluted plants involved in phytoremediation is a big challenge.In this study,nitrogen-doped nanoporous carbon with large specific area of 2359.1 m^(2)g^(-1) is facilely fabricated from metal-polluted miscanthus waste for efficient energy storage.The synergistic effect of KOH,urea and ammonia solution greatly improve the nitrogen quantity and surface area of the synthesized carbon.Electrodes fabricated with this carbon exhibit the excellent capacitance performance of 340.2 F g^(-1) at 0.5 A g^(-1) and a low combined resistance of 0.116Ω,which are competitive with most of previously reported carbon-based electrodes.In addition,the as-obtained carbon electrode shows a high specific capacitance retention of over 99.6%even after 5000 cycles.Furthermore,the symmetric supercapacitor fabricated using the synthesized carbon achieves a superior energy density of 25.3 Wh kg^(-1)(at 400 W kg^(-1))in 1 mol L^(-1) Na_(2)SO_(4)aqueous solution.This work provides an efficient route to upcycle metal-polluted plant waste for supercapacitor applications.
基金supported by the National Natural Science Foundation of China(21476087,21576101)the Innovation Project of Guangdong Department of Education(2014KTSCX016)+1 种基金the Science&Technology Research Project of Guangdong Province(2013B010405005,2014A010105041)the Fundamental Research Funds for the Central Universities~~
文摘Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons(NOMCs) by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy(XPS),cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole(C-PY-900:765 m^2/) and phenanthroline(C-Phen-900:746 m^2/) exhibit higher specific surface areas than the aniline analog(C-PA-900:569 m^2/).Second,the XPS results indicate that the total nitrogen content(ca.3.1–3.3 at%) is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction(ORR).In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.
基金the Open Fund of the Key Laboratory of Enhanced Heat and Energy Conservation of Chinese Ministry of Education, South China University of Technology.
文摘Yellowish nitrogen-doped titania was produced through sol-gel method in mild condition, with the elemental nitrogen derived from aqua ammonia. The titania catalysts were characterized using XRD, BET, TEM, XPS, and UV-Vis diffuse reflectance spectrophotometer, and their photocatalytic activities were evaluated under UV and visible light, respec tively. The XRD results showed that all titania catalysts were anatase. More significantly, the crystallite size of nitrogen-doped titania increased with an increase in N/Ti proportion, and the doping of nitrogen could extend the absorption shoulder into the visible-light region, thus it possessed a higher visible-light activity illustrated by decolorization of methyl orange (65.3%) under the irradiation of visible light, whereas pure titania showed little of such kind of visible light activity. The UV-light activity of nitrogen-doped titania catalysts was worse than that of pure titania and Degussa P25. In the range of N/Ti proportion of 4-10 mol%, the activity of nitrogen-doped titania weakened appreciably in the visible-light region as the N/Ti proportion increased, whereas a reverse relationship existed under the irradiation of UV light.
基金supported by the Scientific and Technological Innovation Platform of Fujian Province(2006L2003)
文摘A novel Ag@nitrogen-doped porous carbon(Ag-NPC) composite was synthesized via a facile hydrothermal method and applied as an anode material in lithium-ion batteries(LIBs). Using this method, Ag nanoparticles(Ag NPs) were embedded in NPC through thermal decomposition of Ag NO_3 in the pores of NPC. The reversible capacity of Ag-NPC remained at 852 m Ah g^(-1)after 200 cycles at a current density of 0.1 A g^(-1), showing its remarkable cycling stability. The enhancement of the electrochemical properties such as cycling performance,reversible capacity and rate performance of Ag-NPC compared to the NPC contributed to the synergistic effects between Ag NPs and NPC.
基金supported by the Synchrotron Light Research Institute(Public Organization)Thailand(GS-54-D01)+7 种基金the Commission on Higher EducationMinistry of EducationThailandperformed under the project"Sustainable Chemical Synthesis(Sus Chem Sys)"which is co-financed by the European Regional Development Fund(ERDF)the state of North Rhine-WestphaliaGermanyunder the Operational Programme"Regional Competitiveness and Employment"2007–2013
文摘Nitrogen-doped carbon nanotubes (NCNTs) were used as a support for iron (Fe) nanoparticles applied in car- bon dioxide (CO_2) hydrogenation at 633 K and 25 bar (1 bar = 10-5 Pa). The Fe/NCNT catalyst promoted with both potassium (K) and manganese (Mn) showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity (GHSV) of 3.1 L-(g·h)-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction (XRD), temperature-programmed reduction (TPR) with molecular hydrogen (H2), and in situ X-ray absorption near-edge structure (XANES) analysis. The Mn pro- moter stabilized wtistite (FeO) as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia (NH_3) decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.
基金financial support from the Ministry of Science and Technology of China(Grants 2016YFB0600901 and 2013CB933100)the National Natural Science Foundation of China(Grants 21573222 and 91545202)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB17020200)financial support from CAS Youth Innovation Promotion(Grant No.2015145)
文摘Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube(N–CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N–CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc–air battery.
基金Supported by the National Natural Science Foundation of China(21401079,21501069)Fundamental Research Funds for Central Universities(JUSRP51626B)+2 种基金the Natural Science Foundation of Jiangsu Province of China(BK20140158,BK20161128,BK20161166)Natural Science Fund for Colleges and Universities in Jiangsu Province(18KJD430008,17KJD430005,17KJB430032)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(PPZY2015B181)
文摘In this paper, nitrogen-doped hierarchical porous carbon(N-HPC) was prepared from polyaniline(PANI)/silica self-aggregates. H-bonding between N\\H groups in aniline/PANI and \\OH groups in nano silica template led to a self-assembly type, which enabled the formation of uniform N-HPC nanoparticles. Silica self-aggregates provided macroporous channels resulted in a decreased diffusion distance. After removing the hard template,the N-HPC had a high surface area(899 m^2·g^(-1)). Owing to two co-existed synergetic energy-storage mechanisms and the hierarchical porous structure, the obtained N-HPC exhibited a high specific capacitance of 218.75 F·g^(-1) at 0.5 A·g^(-1), compared with the nonporous nitrogen-doped carbon(N-C) derived from pure PANI. Moreover, the N-HPC electrode demonstrated excellent cycle life, retaining 99% of its initial specific capacitance after 1000 cycles.
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.