The design and development of porous carbons and their supported Ni-based catalysts, characterized by high activity, stability, and low cost, remain challenging in green chemical processes. In this study, petroleum pitch (PP) and biomass pitch (BP) were employed as inexpensive carbon sources, with polyacrylonitrile (PAN) serving as a texture-modifying agent, to prepare modified carbons (MCs). Porous modified carbons (PMCs) with tailored pore sizes and distributions were comparatively prepared using a nanoscale CaCO3 template and a steam activation method. The results show that pitch-based MCs with a hybrid texture can be produced by mixing 50 wt % PAN with PP or BP, followed by thermal polymerization at 400 degrees C and carbonization at 600 degrees C. Steam activation at 800 degrees C for 1 h enhances pore formation in hybrid MCs derived from PAN-BP compared to those derived from PAN-PP, due to differences in the molecular structures of PP and BP. In contrast, the CaCO3 template method primarily produces mesopores and macropores, whereas steam activation generates abundant micropores and mesopores in PMCs, thereby creating ideal conditions for high-quality catalyst supports. The resulting 10 wt % Ni/PMCBP catalysts demonstrate an impressive phenol conversion of 99.4% and a cyclohexanol selectivity of 94.1% after reaction at 180 degrees C for 2 h, outperforming reference Ni-based catalysts. Additionally, the catalytic performance of phenol hydrogenation is significantly influenced by Ni particle size, which is closely related to the texture and pore characteristics of the carbon supports. This research provides valuable insights into the rational design of PMCs as effective supports for advanced catalytic applications.
Biomass-derived carbons are promising sodium-ion battery anodes because they combine renewable feedstocks, tunable pore structures, and adjustable surface chemistry. However, many biomass carbons still show limited specific capacity and unsatisfactory initial coulombic efficiency. Here, corn silk was used as the carbon precursor, and potassium-sulfate-assisted carbothermal reduction was applied to produce sulfur-enriched porous carbon. Sulfur incorporation introduced C-S-related active sites and high-voltage redox features near 2.1/1.5 V. The optimized SC1400 electrode delivered an initial discharge capacity of 365.94 mAh g-1 at 0.1 A g-1 and an initial coulombic efficiency of 84.52%. It retained 342 mAh g-1 after 500 cycles at 1 A g-1, corresponding to more than 93% capacity retention. The improved cycling stability originates from the coupled effects of a defect-rich framework, enlarged interlayer spacing, and sulfur-containing surface species. Density functional theory calculations are consistent with stronger Na adsorption after sulfur incorporation. Density functional theory calculations support that sulfur incorporation enhances sodium-ion adsorption energy. This work provides a practical route for converting agricultural waste into biomass-derived carbon anodes for sodium-ion batteries.
Biomass-derived carbon materials present significant economic advantages alongside environmental sustainability, owing to their renewable nature and distinctive structure. They have been extensively studied for applications in energy storage. However, the low specific capacity over prolonged cycling periods impedes their progress. Activation of salt templates and heteroatom doping have been proven to be effective methods for enhancing the electrochemical properties of Biomass-derived carbon materials. This study focuses on utilizing waste corn straw as a precursor to develop nitrogen-doped poly porous carbon, which is employed as a negative electrode material for lithium-ion batteries (LIBs). The synergistic effects arising from heteroatom doping coupled with a dual-defect porous carbon structure resulted in exceptional electrochemical performance exhibited by nitrogen-doped corn stover-based porous carbon, achieving a reversible capacity of 425 mAh g(-1) after 600 cycles at a current density of 1 A g(-1). Density functional theory (DFT) calculations corroborate that the incorporation of nitrogen significantly enhances lithium-ion adsorption energies. Through element doping and structural adjustments made within this research, overall electrochemical performances for biomass-derived carbon materials were improved while proposing an economically viable solution for pollution-free sustainable anode materials suitable for industrial-scale production.
N-bromosuccinimide (NBS) has notable selectivity for brominating aromatic compounds with alkyl side chains. This study employs NBS in lieu of liquid bromine to prepare spinnable isotropic pitch derived from ethylene tar pitch (ETP) using a selective photobromination-debromination approach. The prepared isotropic pitches were then utilized to fabricate isotropic pitch-based carbon fibers (IPCFs) through a process involving melt spinning, oxidative stabilization, and subsequent carbonization. As the amount of NBS added increases in the photobromination stage, the softening point, pitch yield, average molecular weight, and degree of polymerization of the resulting isotropic pitch gradually increase, whereas its spinnability first improves but then decreases. Compared with the isotropic pitch manufactured through thermal polymerization alone, the isotropic pitch that undergo photobromination-debromination exhibits a more linear molecular structure formed by methylene/ ethylidene-bridged aromatic units. This molecular structure enhances its spinnability, significantly improving the mechanical performance of the resulting IPCFs. The isotropic pitch produced with 15 wt% NBS during photobromination demonstrates exceptional spinnability, yielding carbon fibers with excellent mechanical characteristics. These fibers exhibit a tensile strength of 1333 MPa, Young's modulus of 64 GPa, and an elongation property of 2.4 %. This work provides a new method for the high value-added utilization of ET by controlling the molecular structure of the pitch precursor.
A metal-organic skeleton (MOF) -derived bimetallic sulfide catalyst, FeCoS2/Fe0.95S1.05, is proposed here for electrochemical ammonia production, which offers a sustainable and energy-saving technical solution for nitrate removal and green NH3 synthesis under environmental conditions. The catalyst benefits from the excellent conductivity and effective synergistic effect of bimetallic sulfides, and it has a NH3 yield of 2.705 mg h- 1 mgcat. - 1 , a maximum Faraday efficiency of 94.79 %, an ammonium selectivity of 96.88 %, and it also maintains good catalytic stability over 12 consecutive cycles. Theoretical and experimental results demonstrate that the incorporation of Fe into the Co site changes the electron configuration of the atoms, resulting in a more pronounced Fe-to-*NO3 electron transfer, and NO3 - can be effectively activated at the surface Fe-Co sites, thereby facilitating the NO3-RR process and realizing efficient NH3 production. Therefore, this study provides a strategy for the design of electrochemical nitrate reduction electrocatalysts.
Nitroaromatic hydrocarbons are commonly converted into aromatic amines using high-pressure hydrogen (H2) in organic solvents over heterogeneous catalysts. However, this method often poses cost challenges and potential risks. Consequently, the careful selection of the reaction medium, hydrogen sources, and efficient catalysts is essential for optimizing production. In this study, a novel mesoporous carbon black-supported nanoscale nickel catalyst, promoted by ruthenium (labeled as Ru-Ni/CB), was developed to reduce nitrobenzene to aniline in an aqueous medium. The results show that the immiscibility of nitrobenzene with water leads to low efficiency when using a 10 wt% Ni/CB catalyst. However, the introduction of a small quantity of Ru, along with specific alcohols, enhances the catalytic reaction by creating a well-miscible ternary phase. A 10 wt% Ru1-Ni9/CB catalyst exhibits exceptional catalytic performance for the hydrogenation of nitrobenzene using both external and endogenous hydrogen. The optimal catalytic coupling effect is achieved through the dehydrogenation of isopropanol and the in-situ hydrogenation of nitrobenzene at 240 degrees C for 2 h, resulting in a 99.0 % conversion of nitrobenzene and a 99.6 % selectivity for aniline. The apparent activation energies for the two tandem reactions are 39.9 and 82.4 kJ/mol, respectively. Furthermore, this catalyst demonstrates superior catalytic performance when compared to many reference catalysts. This study highlights a significant synergistic effect of the Ru-Ni/CB catalyst in nitrobenzene hydrogenation, showcasing high activity, selectivity, and stability.
The homogeneous pore distribution and suitable pore size in porous carbons play a crucial role in enhancing the catalytic performance of carbon-supported catalysts. The strategic design and controllable preparation of porous carbon supports for heterogeneous catalysis still remain a challenge. This study employs a novel method of combining toluene Soxhlet extraction and steam activation to construct homogeneous pores in pitch-based carbon fibers (PCFs) for catalytic applications. The results show that toluene extraction creates abundant micropores in isotropic pitch fibers to form the primary pores, while subsequent steam activation further increases the porosity and pore volume of PCFs. Compared to single methods of toluene extraction or steam activation, this combined approach demonstrates a significant advantage in the design and creation of homogeneous micropores (0.5 similar to 2.0 nm) in PCFs with a high specific surface area of 1169.0 m(2)/g. 10 wt% nanoscale Ni particles supported on the as-prepared porous PCFs exhibit exceptional catalytic performance in the hydrogenation of nitrobenzene to aniline. Under mild reaction conditions of 120 degrees C and 2 h, the conversion of nitrobenzene and the selectivity of aniline approach 96.4 % and 100 %, respectively, superior to those of reference Ni-based catalysts. This work provides a promising strategy for creating homogeneous micropores in PCFs, which are suitable as catalyst supports to achieve the catalytic synthesis of high value-added chemicals.
Glycerol, a major byproduct of biodiesel production, is commonly used as an inexpensive feedstock for hydrogen (H2) production through catalytic reforming. Developing efficient Ni-based catalysts with appropriate supports remains a challenge. In this study, three Ni-based catalysts, each containing 10 wt% Ni with different supports: carbon nanofibers (Ni@CNF), activated carbon (Ni/AC), and alumina (Ni/gamma-Al2O3), were comparatively evaluated for their effectiveness in the catalytic steam reforming of glycerol. The results show that both the catalyst support and the reforming temperature influence the co-production of H2 and carbon nanotubes. All three catalysts exhibit good catalytic performance of H2 production at 700 degrees C for 1 h. The corresponding H2 yields, based on a steam-glycerol molar ratio of 11.9 and a flow rate of 0.2 mL/min, are 86.5%, 81.3%, and 69.2% for Ni@CNF, Ni/AC, and Ni/Al2O3, respectively. Ni@CNF demonstrates high H2 production and good catalytic stability, whereas Ni/Al2O3 generates high-yield carbon nanotubes.
Isotropic pitches with high softening points were controllably synthesized using naphthalene (NAP) via Blanc chloromethylation–dechlorination. Under mild conditions, chloromethyl was introduced into the NAP ring in the presence of chloromethylation reagent. The chloromethylation products of NAP are mainly composed of 1-chloromethylnaphthalene (1-CMNP) and a small amount of 1,4-dichloromethylnaphthalene (1,4-DCMNP). The results of the thermodynamic and kinetic calculations confirmed that the alpha-hydrogen on the NAP ring was more susceptible to being substituted by chloromethyl during chloromethylation, resulting in the formation of 1-CMNP and 1,4-DCMNP. High-quality isotropic pitches with linear methylene-bridged NAP ring structures, characterized by high purity, a high H/C ratio, 100% solubility in quinoline, and excellent spinnability, were obtained after thermal dechlorination polymerization. Due to their homogeneous isotropic phase, appropriate viscosity, and outstanding spinnability, the as-synthesized pitches were adopted as precursors to prepare isotropic pitch-based carbon fibers via melt spinning. Additionally, the investigation of the carbonization behavior of the as-synthesized pitches showed that the naphthalene-derived isotropic pitch obtained at a polymerization temperature of 380 °C had a 57% carbon yield at 800 °C, and its derived semi-cokes displayed an isotropic texture, even when carbonized at 550 °C.
Carbon fibers are one of the most important engineering materials in the current high-tech field. Thus precursors, structure and properties of carbon fibers are necessarily summarized to understand their fundamental principle. Carbonaceous precursors play a decisive role to fabricate advanced carbon fibers. The basic structure of carbon fibers is mostly inherited from the parent precursors and mainly dominates fibers’ physical properties (e.g., strength and modulus), which decide the practical applications. Thereby the morphology, microstructure, crystallite orientation and structure models of various carbon fibers are mainly reviewed. Meanwhile, the size change, new emerging forms and porous functions of carbon fibers and their necessary surface modification are introduced. Finally, the outlook of carbon fibers is briefly presented.
Blanc bromomethylation-dehydrobromination is proposed to synthesize isotropic pitches with superior spinnability, utilizing refined coal tar pitch as the feedstock. This strategy involves introducing bromomethyl functional groups into pitch molecules through the Blanc bromomethylation reaction. In the subsequent process of dehydrobromination, methylene bridges generate between neighboring aromatic molecules. The pitch precursor prepared by this method not only displays an increased level of oligomerization and pitch yield, but also exhibits a more linear molecular structure compared with that produced through purely thermal polycondensation. The enhanced linear molecular configuration contributes to the improved spinnability of the pitch precursor and the oxidation reactivity of its derived fiber. Furthermore, the tensile strength of the resulting carbon fibers rises with an elevation in the amount of polyoxymethylene, and it exhibits the trend of an initial growth followed by a subsequent decrease as the stabilization temperature escalates. The carbon fibers obtained from the pitch prepared through thermal polycondensation present a low Young's modulus of 24 GPa and a low tensile strength measuring of 456 MPa. In contrast, carbon fibers derived from the pitch synthesized via Blanc bromomethylation-dehydrobromination exhibit superior mechanical performance, offering Young's modulus and tensile strength of 58 GPa and 1210 MPa, separately.
The co -carbonization of refined coal tar pitch (RCTP) and brominated industrial methyl naphthalene (BIMNP) employing benzoyl chloride (BC) as a catalyst has been explored to create an isotropic spinnable pitch for carbon fibers with notable tensile strength. BIMNP is derived from industrial methyl naphthalene (IMNP) via photobromination assisted by visible light using N-bromosuccinimide (NBS) as a brominating agent. This research investigates the impact of the mass ratio of RCTP and BIMNP on the composition, molecular structure, and thermophysical characteristics of the co -carbonized pitch. A tentative elucidation of the co -carbonization mechanism involving RCTP, BIMNP, and BC is presented. Adjusting the NBS-to-IMNP mass ratio leads to the complete conversion of 1-methylnaphthalene (1-MNP) and 2-methylnaphthalene (2-MNP) in IMNP into 1-bromomethylnaphthalene (1-BMNP) and 2-bromomethylnaphthalene (2-BMNP), respectively. The co -carbonized pitch exhibits enhanced pitch production, increased thermal stability, and improved spinnability compared to pitch synthesized via thermal polycondensation. The resulting carbon fibers experience a rise in tensile strength by 947 MPa and an increase in Young's modulus by 41.3 GPa as BIMNP content varies from 10% to 30%. Using BIMNP as a co -carbonization agent offers a promising avenue for producing pitch -based carbon fibers meeting automotive industry requirements.
Polyacrylonitrile (PAN)-based composite nanofibers incorporated with high-percentage inexpensive pitch were successfully prepared by a simple electrospinning technique. Low-softening-point naphthalene pitch (NP) has the merit of high solubility but inevitably brings about preoxidation problem. Thus the influence of different preoxidation strategies on the morphology, composition, and structure of composite nanofibers was systematically investigated. The results show that there exists a ternary phase diagram consisting of PAN-pitch-solvent and a suitable apparent viscosity of homogeneous solution, which favors the smooth electrospinning and good adjustment for the diameter of carbon nanofibers (100-500 nm). The crystallinity, crystalline order, and electrical conduction of composite nanofibers are enhanced by incorporating graphitizable NP, for example, the electrical resistance of 50% NP-PAN composite nanofiber films after 800 degrees C carbonization decreases about 30%. Both increasing the oxidation temperature and extending the oxidation time are beneficial to the oxidative stabilization of composite nanofibers with a suitable NP percentage below 50%. Gradient heating (240-340 degrees C) and pressurized (0.08 MPa) preoxidations could accelerate the oxidative stabilization of composite nanofibers with a high NP percentage up to 110% and significantly shorten the oxidation time by half. Therefore, this study paves the road for facile preparation of cost-competitive carbon nanofibers with controllable morphology, structure, and properties.
MXenes are expected to exhibit excellent lithium-ion storage performance due to its good electron conductivity, tunable functional groups, and unique accordion-like structure. However, they suffer from low initial coulombic efficiency (ICE) caused by the trapping and the irreversible reaction between MXene nanosheets and lithium ions. In this work, we propose a facile d-band center regulation strategy via doping engineering to achieve tailorable surface chemistry of MXene, revealing the intrinsic effects of heteroatoms doping on surface chemistry and ICE. This strategy can be applied to various MXenes, which is verified in the case of V2-yCryC as well as TiNbC, and TiVC MXenes. Typically, the V1.8Cr0.2C MXene delivers a double lithium storage capacity in comparison to V2C MXene. Its ICE is improved from 60% to 86%, surpassing most state-of-the-art MXenes. Theoretical calculations reveal that the shift of the d-band center towards the Fermi level is induced by the introduction of Cr and responsible for the improved electrochemical performance. It increases its chemical affinity and absorbability for oxygen-containing functional groups and lithium ions, providing a favorable surface chemistry for efficient lithium storage. This work provides a new strategy to tailor the fine structures of MXenes for their further energy storage applications.
Cyclohexanol is an important feedstock in the chemical industry. Highly selective hydrogenation of phenols to cyclohexanol over non-noble metal catalysts remains a challenge. Herein, four distinctive carbon materials, carbon black (CB), activated carbon (AC), activated carbon fiber (ACF) and carbon nanotube (CNT) were selected as catalyst supports to load Ni nanoparticles for effective phenol hydrogenation. The results show that the phenol conversion and cyclohexanol selectivity in aqueous phase hydrogenation reaction at 180 degrees C for 2 h over 10 wt% Ni/AC catalyst could reach 99.7% and 94.8%, respectively. These values are better than those obtained over 10 wt% Ni/ACF, Ni/CNT and Ni/Al2O3. After surface modification of carbon supports, the catalytic activity and reuse effect of modified catalysts are significantly enhanced and the optimal temperature decreases to 150 degrees C. This is because that modified carbon supports have abundant surface functional groups so as to provide a high dispersion and stable anchor of ultrafine active Ni nanoparticles (-12 nm). Phenol hydrogenation catalyzed by different Ni/carbon catalysts conforms to a first-order reaction, and their apparent activation energies are in a range of 49-68 kJ mol- 1 (49 corresponds to the modified catalyst Ni/MAC), which are markedly lower than that of Ni/Al2O3 (-96 kJ mol- 1). The potential mechanism of highly selective hydrogenation of phenol to cyclohexanol in this work is mainly controlled by the reaction kinetics, which is closely related to the different desorption abilities of cyclohexanone and cyclohexanol from the catalysts.
Ni-based catalysts are increasingly being used in nitrobenzenehydrogenation. How to select suitable catalyst supports is crucialfor upgrading the catalytic performance. Herein, three Ni-based catalystssupported on activated carbon fiber (ACF), mesoporous carbon black(CB), and & gamma;-Al2O3 were tested for nitrobenzenehydrogenation. The influence of catalyst supports, their porositycharacteristics, and reaction conditions on the catalytic performancewas investigated. The results show that 10 wt % Ni/CB catalyst ownsan ultrafine active Ni nanoparticles (& SIM;10 nm) with a uniformdispersion and thus exhibits the optimal catalytic activity. The conversionof nitrobenzene and the selectivity to aniline could reach nearly100% at 120 & DEG;C for 1 h. By contrast, it takes 2 h to achievethe same conversion for 10 wt % Ni/ACF at 120 & DEG;C, whereas 10wt % Ni/Al2O3 needs a severe reaction at 150 & DEG;C for 2 h. The turnover frequency of 10 wt % Ni/CB approaches38 h(-1), which is higher than those of other catalysts.Nitrobenzene hydrogenation over different catalysts conforms to afirst-order reaction, and the apparent activation energy of 10 wt% Ni/CB (42.6 kJ/mol) is significantly lower than that of 10 wt %Ni/Al2O3 (66.0 kJ/mol). Moreover, 10 wt % Ni/CBcatalyst exhibits a good recyclability and structural stability owingto the existence of abundant mesopores in CB, in comparison with 10wt % Ni/ACF and Ni/Al2O3. It is the mesoporesrather than the micropores in carbon supports to postpone the deactivationof Ni-based catalysts. This work demonstrates the superiority of porouscarbons as catalyst supports over Al2O3 in nitrobenzenehydrogenation.
In situ derivation of TiO2 from Ti2CTx and Ti3C2Tx MXenes is a promising strategy to construct TiO2-based heterostructure. How to precisely control the conversion depth of MXene and well maintain its lamellar structure are the top priority. Herein, double transition metal (Ti, V) MXenes (Ti2-yVyCTx) act as precursors to engineer TiO2/MXene heterostructure as anode materials for lithium-ion batteries. Due to the different oxidation tendency, vanadium atoms with higher oxidative tolerance can maintain the 2D lamella morphology and high electronic conductivity while titanium atoms can be selectively oxidized to well-dispersed TiO2 nanoparticles. Moreover, the content and dispersity of derived TiO2 nanoparticles can be well controlled by adjusting the molar ratio of Ti/V in the Ti2-yVyCTx precursors. The intensive interfacial interaction between derived TiO2 and vanadium dominated MXene layers protects TiO2 nanoparticles from pulverization and detachment from 2D MXene as well as the restacking of MXene layers during charge/discharge cycles. Benefiting from the synergistic effects, the TiO2@TiVCTx anode delivers a superior specific capacity of 741.2 mAh g-1 at 0.1 A g-1, which shows prominent advantage in current MXene-derived anode materials. This work innovatively realizes atomically selective oxidation of double metal transition MXenes and regulate the derivatives for high performance anode materials.
Transition metal nanoparticles supported on porous carbon materials as hydrothermal stable and highly effective catalysts are increasingly attracting worldwide attention. Herein, a controllable electrospinning technique was employed to prepare the promising catalysts to produce hydrogen. Different proportions of polymethyl methacrylate and nickel nitrate were introduced into polyacrylonitrile spinning solution to prepare nano scale Ni encapsulated in porous carbon nanofiber (Ni@PCNF) through an in-situ pore making strategy. The results show that the prepared 10 wt% Ni@PCNF catalyst possesses an enhanced specific surface area, hierarchical porous structure, and uniformly-dispersed Ni nanoparticles (-17 nm). This porous and fibrous catalyst presents relatively high performance of producing high-purity H2 by aqueous phase reforming of glycerol compared with several reference catalysts on different supports (e.g., activated carbon fibers and g-Al2O3) under similar reaction conditions. The selectivity and purity of H2 produced by 10 wt % Ni@PCNF catalyst at 260 degrees C for 1 h are nearly 100% and 93%, respectively. This is related to the moderate catalytic activity of active Ni nanoparticles encapsulated in PCNFs. By contrast, those Ni nanoparticles supported on the reference supports show a high catalytic activity and thus produce low-purity H2 due to the considerable byproducts of CH4, CO and CO2. Moreover, Ni@PCNF catalyst exhibits a good structure stability and reuse effect in comparison with reference catalysts. This work provides a roadmap for preparing effective and stable Ni-based catalysts to produce high-purity H2 from cheap glycerol through a low temperature thermocatalysis. (c) 2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Ferroferric oxide (Fe3O4) as an anode material of lithium-ion battery has been widely investigated due to its high theoretical capacity, environmental friendliness, natural abundance, and low cost. However, it suffers from severe aggregation and volume expansion during energy storage. Herein, we rationally construct an advanced Fe2N@Fe3O4/VN heterostructure via a hydrothermal and followed nitridation process, where the wrapping of conductive Fe2N on the surface of Fe3O4 effectively improves the electron conductivity and alleviates the volume expansion, and VN inhibits the agglomeration of Fe2N@Fe3O4. Benefiting from the dual conductive confinements and promoted interfacial charge transfer, the Fe2N@Fe3O4/VN heterojunction exhibits excellent rate capability and cycling stability. It possesses the highest reversible capacity of 420.8 mAh g-1 at 1 A g-1 after 600 cycles, which is three times that of Fe3O4. Furthermore, a full cell based on a Fe2N@Fe3O4/VN anode and a LiFePO4 cathode delivers considerable electrochemical performance. This work demonstrates that Fe2N@Fe3O4/VN is a potential anode material and provides a model in constructing other high-performance electrode materials.
Hard carbon is regarded as a promising anode material for sodium/potassium-ion batteries, which have attracted much attention in grid-scale energy storage. However, it still suffers from the sluggish electrochemical kinetics rooted in the turbostratic structure of carbon, leading to an inferior rate capacity. Herein we utilize a facile strategy to fabricate the edge-enriched and S-doped carbon nanorods (SCNs) with controllable diameter and highly-oriented carbon layer arrangement. The abundant edges lead to the shorter diffusion path of ions, as well as the enlarged layer spacing, both contribute to the rapid kinetics of ionic insertion/desertion. Such a unique highly-oriented structure enables the SCNs anodes to deliver excellent rate capacities and long-lasting cycling life for both sodium and potassium ion storage. The density functional theory (DFT) results demonstrate the enhanced adsorption and reduced ions diffusion energy barrier of Na+ ions near the S-doped active sites, which substantiates the promoted electrochemical kinetics of SCNs electrodes. This work inspires more ideas for rational design of advanced electrodes and provides an in-depth insight into the reaction kinetics of carbonaceous anodes.