Nitrogen-doped hierarchical porous carbon from polyaniline/silica self-aggregates for supercapacitor

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.

Nitrogen-doped porous carbon nanosheets as both anode and cathode for advanced potassium-ion hybrid capacitors

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.

PtZn nanoparticles supported on porous nitrogen-doped carbon nanofibers as highly stable electrocatalysts for oxygen reduction reaction

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.

Hierarchically porous nitrogen-doped carbon as cathode for lithium–sulfur batteries

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.

Novel Ag@Nitrogen-doped Porous Carbon Composite with High Electrochemical Performance as Anode Materials for Lithium-ion Batteries

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.

Controllable synthesis of nitrogen-doped porous carbon from metal-polluted miscanthus waste boosting for supercapacitors

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.

Nitrogen-doped hierarchical few-layered porous carbon for efficient electrochemical energy storage

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.

Nitrogen-doped hierarchically porous carbon spheres for low concentration CO_(2) capture

Synthesis of spherical carbon beads with effective CO_2 capture capability is highly desirable for large scale application of CO2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare nitrogen-doped hierarchically porous carbon spheres was developed via co-pyrolyzation of poly(vinylidene chloride) and melamine in alginate gel beads. In this approach, melamine not only serves as the nitrogen precursor, but also acts as a template for the macropores structures. The nitrogen contents in the hierarchically porous carbon spheres reach a high level, ranging from 11.8 wt% to 14.7 wt%, as the melamine amount increases. Owing to the enriched nitrogen functionalities and the special hierarchical porous structure, the carbon spheres exhibit an outstanding CO_2 capture performance, with the dynamic capacity of as much as about 7 wt% and a separation factor about 49 at 25 °C in a gas mixture of CO_2/N_2(0.5:99.5, v/v).

Red-blood-cell-like nitrogen-doped porous carbon as an efficient metal-free catalyst for oxygen reduction reaction

A red-blood-cell-like nitrogen-doped porous carbon catalyst with a high nitrogen content(9.81%)and specific surface area(631.46 m^2/g)was prepared by using melamine cyanuric acid and glucose as sacrificial template and carbon source,respectively.This catalyst has a comparable onset potential and a higher diffusion-limiting current density than the commercial 20 wt%Pt/C catalyst in alkaline electrolyte.The oxygen reduction reaction mechanism catalyzed by this catalyst is mainly through a 4e pathway process.The excellent catalytic activity could origin from the synergistic effect of the in-situ doped nitrogen(up to 9.81%)and three-dimensional(3D)porous network structure with high specific surface area,which is conducive to the exposure of more active sites.It is interesting to note that the catalytic activity of oxygen reduction strongly depends on the proportion of graphic N rather than the total N content.

Ultra-stable and High-rate Lithium Ion Batteries Based on Metal-organic Framework-derived ln2O3 Nanocrystals/Hierarchically Porous Nitrogen-doped Carbon Anode

Exploring electrode materials with attractive specific capacity and prominent cyclic durability is of the essence for promoting lithium ion batteries(LIBs).In2O3 has shown an extraordinary promise for LIBs with advantageous gravimetric capacity(theoretically 965 mA h g-1) and low working voltage.However,In2O3 still suffers from the inherent weaknesses of metal oxides in practical application,especially low conductivity and incorrigible volume expansion upon the cycling process.Here,we demonstrate the architecture of metal-organic framework(MOF)-derived In2O3 nanocrystals/hierarchically porous nitrogen-doped carbon composite(In2O3/HPNC) for ultra-stable LIBs anode.This hierarchically porous structure(micro/meso/macro-pores) with nitrogen doping not only ensures exceptional mechanical strength and accommodates the volume expansion of In2O3 nanocrystals,but also offers electrons and lithium ions efficient interpenetrating pathways to migrate rapidly during charge/discharge processes.Thus,In2O3/HPNC exhibits excellent cyclic stability with a high specific capacity of 623 mA h g-1 over2000 cycles at 1000 mA g-1,corresponding to an ultra-low specific capacity decay of 0.017% per cycle(the best among the ln203-based anode for LIBs),and outstanding rate performance,suggesting a critical step toward achieving long-life and high-rate LIBs in practical devices.

Tailoring the Porous Structure of Mono-dispersed Hierarchically Nitrogen-doped Carbon Spheres for Highly Efficient Oxygen Reduction Reaction

The search for a low-cost metal-free cathode material with excellent mass transfer structure and catalytic activity in oxygen reduction reaction(ORR)is one of the most challenging issues in fuel cells.In this work,nitrogen-rich mphenylenediamine is introduced into the synthesis of porous carbon spheres to tune the pore structure and nitrogen-doped active sites.As a result,more pyridinic N and pyrrolic N functional species were observed at the interior and surface of the carbon spheres.The introduction of m-phenylenediamine also regulated the nucleating of precursors,an urchin-like mesoporous surface structure ensures point contact and less agglomeration between each particle was obtained.With optimized proportion of micropores/mesopores and improved nitrogen-contained functional species,the ORR activity can be remarkably improved.The half-wave potential of this catalyst could achieve to 0.81 V(versus RHE)which is only 42 m V lower than commercial Pt/C catalyst.Furthermore,the optimized cathode catalyst achieved a 69 m W cm-2 maximum power density when operated in direct methanol fuel cells at room temperature.

CoN_(x)C active sites-rich three-dimensional porous carbon nanofibers network derived from bacterial cellulose and bimetal-ZIFs as efficient multifunctional electrocatalyst for rechargeable Zn–air batteries

In this work, a CoNxC active sites-rich three-dimensional porous carbon nanofibers network derived from bacterial cellulose and bimetal-ZIFs is prepared via a nucleation growth strategy and a pyrolysis process.The material displays excellent electrocatalytic activity for the oxygen reduction reaction, reaching a high limiting diffusion current density of -7.8 mA cm^(-2), outperforming metal–organic frameworks derived multifunctional electrocatalysts, and oxygen evolution reaction and hydrogen evolution reaction with low overpotentials of 380 and 107 mV, respectively. When the electrochemical properties are further evaluated, the electrocatalyst as an air cathode for Zn-air batteries exhibits a high cycling stability for63 h as well as a maximum power density of 308 mW cm^(-2), which is better than those for most Zn-air batteries reported to date. In addition, a power density of 152 mW cm^(-2) is provided by the solid-state Zn-air batteries, and the cycling stability is outstanding for 24 h. The remarkable electrocatalytic properties are attributed to the synergistic effect of the 3 D porous carbon nanofibers network and abundant inserted CoNxC active sites, which enable the fast transmission of ions and mass and simultaneously provide a large contact area for the electrode/electrolyte.

Hydrogel-derived nitrogen-doped porous carbon framework with vanadium nitride decoration for supercapacitors with superior cycling performance

Transition metal nitrides(TMNs)and their composites with carbon materials hold tremendous potential for supercapacitor(SC)electrodes because of their excellent electronic conductivity and electrochemical activity.However,realizing cycling stable TMN/carbon-based supercapacitors with economically viable and environmentally-friendly approaches remains a significant challenge.Significantly,polyacrylamide(PAM)hydrogel,as a water-soluble linear polymer electrolyte,is expected to be a remarkable candidate precursor for preparing N-doped porous carbon(NPC)due to the high contents of carbon and nitrogen elements.In this study,vanadium nitride(VN)embedded in PAM hydrogel-derived NPC was fabricated successfully via an ammonia-free process.The VN/NPC delivers a high specific capacitance of 198.3 F g^(−1)at a current density of 1 A g^(−1),with a remarkable cycling stability of 107%after 16,000 cycles.The electrochemical performances of VN/NPC compared to bare VN nanoparticles are strongly improved due to the composite structure.Additionally,the VN/NPC-based solid-state symmetric device delivers an excellent energy density of 21.97µWh cm^(−2)at a power density of 0.5 mW cm^(−2),and an outstanding cycling durability of 90.9%after 18,000 cycles.This work paves the way to design metal nitride/porous carbon materials,which also opens up unique horizons for the recovery of hydrogel electrolyte.

Nitrogen-doped porous carbons from polyacrylonitrile fiber as effective CO_(2) adsorbents

In this report, nitrogen-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile two-step synthesis process i.e. carbonization followed by KOH activation. Activation temperature and KOH/carbon ratio are two parameters to tune the porosity and surface chemical properties of sorbents. The as-obtained sorbents were carefully characterized.Special attention was paid concerning the change of sorbents’ morphology with respect to synthesis conditions. Under the activation temperatures of this study, the sorbents can still retain their fibrous structure when the KOH/carbon mass ratio is 1. Further increasing the KOH amount will destroy the original morphology of polyacrylonitrile fiber. CO_(2)adsorption performance tests show that a sorbent retaining the fibrous shape possesses the highest CO_(2)uptake of 3.95 mmol/g at 25℃and 1 bar. Comprehensive investigation found that the mutual effect of narrow microporosity and doped N content govern the CO_(2)adsorption capacity of these adsorbents. Furthermore, these polyacrylonitrile fiber-derived carbons present multiple outstanding CO_(2)capture properties such as excellent recyclability, high CO_(2)/N_(2)selectivity, fast adsorption kinetics, suitable heat of adsorption, and good dynamic adsorption capacity. Hence, nitrogen-doped porous carbons with fibrous structure are promising in CO_(2)capture.

Template-assisted formation of atomically dispersed iron anchoring on nitrogen-doped porous carbon matrix for efficient oxygen reduction

Isolated active metal atoms anchored on nitrogen-doped carbon matrix have been developed as the efficient catalyst for accelerating sluggish reaction kinetics of oxygen reduction reaction(ORR).The facile rational structure engineering with abundant isolated active metal atoms is highly desirable but challenging.Herein,we demonstrate that atomically dispersed Fe sites(Fe-N4 moieties)on the hierarchical porous nitrogen-doped carbon matrix(Fe-SA-PNC)for high ORR activity can be achieved by a dual-template assisted strategy.By thermal decomposition of NH_(4)Cl template,the nitrogen-doped carbon matrix is generated based on the interaction with carbon precursor of citric acid.Meanwhile,the introduction of NaCl template facilitates the formation of hierarchical porous structures,which enable more active sites exposed and improve the mass transfer.Interestingly,the dual-template strategy can inhibit the formation of iron carbide nanoparticles(NPs)by generating porous structures and avoiding of the rapid loss of nitrogen during pyrolysis.The as-made Fe-SA-PNC catalysts with well-defined Fe-N_(4)active sites exhibit highly efficient ORR activity with a half-wave potential of 0.838 V versus the reversible hydrogen electrode,as well as good stability and methanol tolerance,outperforming the commercial Pt/C.The zinc-air battery(ZAB)constructed by Fe-SA-PNC also shows a higher peak power density and specific discharging capacity than that of Pt-based ZAB.The present work provides the facile strategy for tailoring nitrogen doping and porous structures simultaneously to prevent the formation NPs for achieving the well-dispersed and accessible single-atom active sites,paving a new way to design efficient electrocatalysts for ORR in fuel cells.

Effect of carbonization atmosphere on electrochemical properties of nitrogen-doped porous carbon

Nitrogen atom doping has been found to enhance the electrochemical performance of porous carbon(PC).In this study,hollow tubular nitrogen-doped porous carbon(N/PC)was synthesized using polyvinylpyrrolidone as the carbon–nitrogen source and fibrous brucite as the template through carbonization.The effects of nitrogen and argon protective atmospheres on the nitrogen content,the specific surface area(SSA),and electrochemical properties of N/PC were investigated.The results showed that compared with N/FBC-Ar,N/FBC-N2 prepared in nitrogen protective atmosphere had a higher nitrogen content and a larger proportion of pyrrolic nitrogen(N-5)and pyridinic nitrogen(N-6).N/FBC-N2 displayed a specific capacitance(C)of 194.1 F·g^(−1)at 1 A·g^(−1),greater than that of N/FBC-Ar(174.3 F·g^(−1)).This work reveals that the nitrogen doping with a higher nitrogen content in nitrogen protective atmosphere is more favorable.Furthermore,a larger proportion of pyrrolic nitrogen and pyridinic nitrogen in the doped nitrogen atoms significantly enhances the electrochemical performance.

Nitrogen-doped carbon nanotube/polyaniline composite:Synthesis, characterization, and its application to the detection of dopamine

Nitrogen-doped carbon nanotubes (N-CNTs)/polyaniline (PANI) composites are developed as an electrode material for biosensors. The morphology, composition, and optical properties of the resulting products were characterized by transmission electron microscopy (TEM), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FT-IR), and ultraviolet-visible absorption spectra (UV-vis). Furthermore, N-CNTs/PANI composite was immobilized on the surface of a glassy carbon electrode (GCE) and applied to construct a sensor. The obtained N-CNTs/PANI-modified GCE showed one pair of redox peaks and high catalytic activity for the oxidation of dopamine (DA) in a neutral environment. Differential pulse voltam-mograms results illustrate that the fabricated DA biosensor has high anti-interference ability towards ascorbic acid (AA). In addition, the fabricated biosensor showed superior performances with two wide linear ranges from 1 to 80 μM and from 1.5 to 3.5 mM and a low detection limit of 0.01 μM.

NiRh nanoparticles supported on nitrogen-doped porous carbon as highly efficient catalysts for dehydrogenation of hydrazine in alkaline solution

Well-dispersed bimetallic NiRh nanoparticles （NPs） with different compositions supported on nitrogen-doped porous carbon （NPC） derived from metal-organic frameworks （ZIF-8） were synthesized through a co-reduction method. The NPC-900 supported NiRh catalyst exhibits the highest catalytic activity and 100% hydrogen selectivity toward hydrogen generation from hydrazine. These properties might be attributed to the high surface area and high graphitization of the NPC. This strategy may open up a new avenue for designing high-performance catalysts by utilizing NPC as a support to anchor active metal NPs for additional applications.

Development of N-doped carbons from zeolite-templating route as potential electrode materials for symmetric supercapacitors

N-doped carbons were fabricated from zeolite-templated carbon via modification with melamine and mild KOH activation. The N-doping treatment and KOH activation slightly lowered the surface areas of pristine zeolite-templated carbon; nonetheless, N-doped carbons with a lower surface area exhibited much higher capacitance and cycling stability as fabricated into symmetric supercapacitor. Significantly, N-doped carbon obtained at 700°C showed a capacitance of 45.7 F/g at 0.1 A/g and 42.0 F/g at 10 A/g for the fabricated supercapacitor with 6 M KOH electrolyte, with 92% retention of initial capacitance as current density increased up to 100-fold. This performance was attributed to the dual contribution of electric double-layer capacitance and pseudo-capacitance. The assembled supercapacitor also exhibited excellent cycling stability, with 91% capacitance retention at 10 A/g after 10000 cycles.

Nitrogen-doped porous carbon nanofoams with enhanced electrochemical kinetics for superior sodium-ion capacitor

Many electrochemical energy storage devices,such as batteries,supercapacitors,and metal ion capacitors,rely on effective and inexpensive electrode materials.Herein,we have developed highly active nitrogen-doped porous carbon nanofoams(NPCNs-600-N)for sodium-ion capacitors(SICs).NPCNs-600-N have a highly porous framework,extended interlayer spacing(0.41 nm),and lots of surface functional groups.Accordingly,NPCNs-600-N achieves a high reversible capacity(301 mAh·g^(-1)at 0.05 A·g^(-1)),superior rate capability(112 mAh·g^(-1)at 5.00 A·g^(-1)),and ultra-stable cyclability.The excellent rate and cycling performance originate from the abundant active sites and porous architecture of NPCNs-600-N.Further-more,SICs device is constructed by employing the NPCNs-600-N as the battery-like anode and commercial superconductive carbon black as the capacitive cathode,which delivers high energy/power densities of 92 Wh·kg^(-1)/15984 W·kg^(-1)with a remarkable cyclability(93%reten-tion over 5000 cycles at 1.00 A·g^(-1)).The methodology of the work enables the simultaneous tuning of the porous architectures and surface function groups of carbon for high-performance SICs.