MOF-derived porous graphitic carbon with optimized plateau capacity and rate capability for high performance lithium-ion capacitors

The development of anode materials with high rate capability and long charge-discharge plateau is the key to improve per-formance of lithium-ion capacitors(LICs).Herein,the porous graphitic carbon(PGC-1300)derived from a new triply interpenetrated co-balt metal-organic framework(Co-MOF)was prepared through the facile and robust carbonization at 1300°C and washing by HCl solu-tion.The as-prepared PGC-1300 featured an optimized graphitization degree and porous framework,which not only contributes to high plateau capacity(105.0 mAh·g^(−1)below 0.2 V at 0.05 A·g^(−1)),but also supplies more convenient pathways for ions and increases the rate capability(128.5 mAh·g^(−1)at 3.2 A·g^(−1)).According to the kinetics analyses,it can be found that diffusion regulated surface induced capa-citive process and Li-ions intercalation process are coexisted for lithium-ion storage.Additionally,LIC PGC-1300//AC constructed with pre-lithiated PGC-1300 anode and activated carbon(AC)cathode exhibited an increased energy density of 102.8 Wh·kg^(−1),a power dens-ity of 6017.1 W·kg^(−1),together with the excellent cyclic stability(91.6%retention after 10000 cycles at 1.0 A·g^(−1)).

Piezoresistivity of Carbon Fiber Graphite Cement-based Composites with CCCW

The electrical conductivity and piezoresistivity of carbon fiber graphite cement-matrix composites（CFGCC） with carbon fiber content（1% by the weight of cement）,graphite powder contents （0%-50% by the weight of cement） and CCCW（cementitious capillary crystalline waterproofing materials,4% by the weight of cement） were studied.The experimental results showed that the relationship between the resistivity of CFGCC and the concentration of graphite powders had typical features of percolation phenomena.The percolation threshold was about 20%.A clear piezoresistive effect was observed in CFGCC with 1wt% of carbon fibers,20wt% or 30wt% of graphite powders under uniaxial compressive tests,indicating that this type of smart composites was a promising candidate for strain sensing.The measured gage factor （defined as the fractional change in resistance per unit strain） of CFGCC with graphite content of 20wt% and 30wt% were 37 and 22,respectively.With the addition of CCCW,the mechanical properties of CFGCC were improved,which benefited CFGCC piezoresistivity of stability.

Highly N-doped carbon with low graphitic-N content as anode material for enhanced initial Coulombic efficiency of lithium-ion batteries

N-doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li+storage performance.However,N-doped carbon anodes still suffer from low N-doping levels and low initial Coulombic efficiency(ICE).In this study,high N-doped and low graphitic-N carbons(LGNCs)with enhanced ICE were synthesized by taking advantage of a denitrification strategy for graphitic carbon nitride(g-C_(3)N_(4)).In brief,more than 14.5 at%of N from g-C_(3)N_(4)(55.1 at%N)was retained by reacting graphitic-N with lithium,which was subsequently removed.As graphitic-N is largely responsible for the irreversible capacity,the anode's performance was significantly increased.Compared to general N-doped carbons with high graphitic-N proportion(>50%)and low N content(<15 at%),LGNCs delivered a low proportion of 10.8%-17.2% within the high N-doping content of 14.5-42.7 at%,leading to an enhanced specific capacity of 1499.9mAh g^(-1) at an ICE of 93.7% for the optimal sample of LGNC(4:1).This study provides a facile strategy to control the N content and speciation,achieving both high Li+storage capacity and high ICE,and thus promoting research and application of N-doped carbon materials.

Composite polymer electrolyte reinforced by graphitic carbon nitride nanosheets for room-temperature all-solid-state lithium batteries

By virtue of the flexibility and safety, polyethylene oxide(PEO) based electrolytes are regarded as an appealing candidate for all-solid-state lithium batteries. However, their application is limited by the poor ionic conductivity at room temperature, narrow electrochemical stability window and uncontrolled growth of lithium dendrite. To alleviate these problems, we introduce the ultrathin graphitic carbon nitride nanosheets(GCN) as advanced nanofillers into PEO based electrolytes(GCN-CPE). Benefiting from the high surface area and abundant surface N-active sites of GCN, the GCN-CPE displays decreased crystallinity and enhanced ionic conductivity. Meanwhile, Fourier transform infrared and chronoamperometry studies indicate that GCN can facilitate Li+migration in the composite electrolyte. Additionally, the GCN-CPE displays an extended electrochemical window compared with PEO based electrolytes. As a result, Li symmetric battery assembled with GCN-CPE shows a stable Li plating/stripping cycling performance, and the all-solid-state Li/LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622) batteries using GCN-CPE exhibit satisfactory cyclability and rate capability in a voltage range of 3-4.2 V at 30 ℃.

Extraordinary Ultrahigh-Capacity and Long Cycle Life Lithium-Ion Batteries Enabled by Graphitic Carbon Nitride-Perylene Polyimide Composites

Graphitic carbon nitride(g-C_(3)N_(4))is widely used in organic metal-ion batteries owing to its high porosity,facile synthesis,stability,and high-rate performance.However,pristine g-C_(3)N_(4)nanosheets exhibit poor electrical conductivity,irreversible metal-ion storage capacity,and short-term cycling owing to their high concentration of graphitic-N species.Herein,a series of 3,4:9,10-perylenetetracarboxylic diimide-coupled g-C_(3)N_(4)composite anode materials,CN-PI_(x)(x=0.2,0.5,0.75,and 1),was investigated,which exhibited an unusually high surface nitrogen content(23.19-39.92 at.%)and the highest pyridinic-N,pyrrolic-N,and graphitic-N contents reported to date.The CN-PI_(1)anode delivers an unprecedented and continuously increasing ultrahigh discharging capacity of exceeding 8400 mAh g^(-1)(1.96 mWh cm^(-2))at 100 mA g^(-1)with high specific energy density(E_(sp))of~7700 Wh kg^(-1)and the volumetric energy density(E_(v))of~14956 Wh L-1 and an excellent long-term stability(414 mAh g^(-1)or 0.579 mWh cm^(-2)at 1 A g^(-1)).Furthermore,the activation of the CN-PI_(x)electrodes contributes to their superior electrochemical performance,resulting from the fact that the Li+is not only stored in the CN-PI_(x)composites but also CN-PI_(x)activated the Li^(0)adlayer on the CN-PI_(1)-Cu heterojunction as an SEI layer to avoid the direct contact of Li^(0)phase and the electrolyte.The CN-PI_(1)full cell with LiCoO_(2)as the cathode delivers a discharge capacity of~587 mAh g^(-1)at a 1 A g^(-1)after 250 cycles with a Coulombic efficiency nearly 99%.This study provides a strategy to develop N-doped g-C_(3)N_(4)-based anode materials for realizing long-lasting energy storage devices.

Smart Interfacing between Co-Fe Layered Double Hydroxide and Graphitic Carbon Nitride for High-efficiency Electrocatalytic Nitrogen Reduction

Bimetallic compounds such as hydrotalcite-type layered double hydroxides(LDHs)are promising electrocatalysts owing to their unique electronic structures.However,their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled,electronegative-OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules.Herein,a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C_(3)N_(4),which is proven by density functional theory(DFT)investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface.The interfaced LDH and g-C_(3)N_(4) is further hybridized with a self-standing TiO_(2) nanofibrous membrane(NM)to maximize the interfacial effect owing to its high porosity and large surface area.Profited from the synergistic superiorities of the three components,the LDH@C_(3)N_(4)@TiO_(2) NM delivers superior ammonia yield(2.07×10^(−9) mol s^(−1) cm^(−2))and Faradaic efficiency(25.3%),making it a high-efficiency,noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.

Engineering g-C_(3)N_(4)based materials for advanced photocatalysis:Recent advances

Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.

Recent Advances of Graphitic Carbon Nitride-Based Structures and Applications in Catalyst, Sensing, Imaging, and LEDs

The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of environmental remediation. The g-C_3N_4-based materials have excellent electronic band structures, electron-rich properties, basic surface functionalities, high physicochemical stabilities and are ‘‘earth-abundant.'' This review summarizes the latest progress related to the design and construction of g-C_3N_4-based materials and their applications including catalysis, sensing,imaging, and white-light-emitting diodes. An outlook on possible further developments in g-C_3N_4-based research for emerging properties and applications is also included.

Effect of the graphitic degree of carbon supports on the catalytic performance of ammonia synthesis over Ba-Ru-K/HSGC catalyst

A series of high surface area graphitic carbon materials （HSGCs） were prepared by ball-milling method. Effect of the graphitic degree of HSGCs on the catalytic performance of Ba-Ru-K/HSGC-x （x is the ball-milling time in hour） catalysts was studied using ammonia synthesis as a probe reaction. The graphitic degree and pore structure of HSGC-x supports could be successfully tuned via the variation of ball-milling time. Ru nanoparticles of different Ba-Ru-K/HSGC-x catalysts are homogeneously distributed on the supports with the particle sizes ranging from 1.6 to 2.0 nm. The graphitic degree of the support is closely related to its facile electron transfer capability and so plays an important role in improving the intrinsic catalytic performance of Ba-Ru-K/HSGC-x catalyst.

Monolayer Graphitic Carbon Nitride as Metal-Free Catalyst with Enhanced Performance in Photo- and Electro-Catalysis

The exfoliation of bulk graphitic carbon nitride(g-C_(3)N_(4))into monolayer has been intensively studied to induce maximum sur-face area for fundamental studies,but ended in failure to realize chemi-cally and physically well-defined monolayer of g-C_(3)N_(4)mostly due to the difficulty in reducing the layer thickness down to an atomic level.It has,therefore,remained as a challenging issue in two-dimensional(2D)chemistry and physics communities.In this study,an“atomic monolayer of g-C_(3)N_(4)with perfect two-dimensional limit”was successfully prepared by the chemically well-defined two-step routes.The atomically resolved monolayer of g-C_(3)N_(4)was also confirmed by spectroscopic and micro-scopic analyses.In addition,the experimental Cs-HRTEM image was collected,for the first time,which was in excellent agreement with the theoretically simulated;the evidence of monolayer of g-C_(3)N_(4)in the perfect 2D limit becomes now clear from the HRTEM image of orderly hexagonal symmetry with a cavity formed by encirclement of three adjacent heptazine units.Compared to bulk g-C_(3)N_(4),the present g-C_(3)N_(4)monolayer showed significantly higher photocatalytic gen-eration of H2O2 and H2,and electrocatalytic oxygen reduction reaction.In addition,its photocatalytic efficiency for H2O2 production was found to be the best for any known g-C_(3)N_(4)nanomaterials,underscoring the remarkable advantage of monolayer formation in optimizing the catalyst performance of g-C_(3)N_(4).

Highly Dispersed Cobalt Nanoparticles Embedded in Nitrogen-Doped Graphitized Carbon for Fast and Durable Potassium Storage

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.

FeCo alloy@N-doped graphitized carbon as an efficient cocatalyst for enhanced photocatalytic H2 evolution by inducing accelerated charge transfer

Cocatalysts play important roles in improving the activity and stability of most photocatalysts.It is of great significance to develop economical,efficient and stable cocatalysts.Herein,using Na2CoFe(CN)6 complex as precursor,a novel noble-metal-free FeCo@NGC cocatalyst(nano-FeCo alloy@N-doped graphitized carbon) is fabricated by a simple pyrolysis method.Coupling with g-C3 N4, the optimal FeCo@NGC/g-C3N4 receives a boosted visible light driven photocatalytic H2 evolution rate of 42.2 μmol h-1, which is even higher than that of 1.0 wt% Pt modified g-C3N4 photocatalyst.Based on the results of density functional theory(DFT) calculations and practical experiment measurements,such outstanding photocatalytic performance of FeCo@NGC/g-C3N4 is mainly attributed to two aspects.One is the accelerated charge transfer behavior,induced by a photogene rated electrons secondary transfer performance on the surface of FeCo alloy nanoparticles.The other is related to the adjustment of H adsorption energy(approaching the standard hydrogen electrode potential) by the presence of external NGC thin layer.Both factors play key roles in the H2 evolution reaction.Such outstanding performance highlights an enormous potential of developing noble-metal-free bimetallic nano-alloy as inexpensive and efficient cocatalysts for solar applications.

Band Engineering and Morphology Control of Oxygen‑Incorporated Graphitic Carbon Nitride Porous Nanosheets for Highly Efficient Photocatalytic Hydrogen Evolution

Graphitic carbon nitride(g-C3N4)-based photocatalysts have shown great potential in the splitting of water.However,the intrinsic drawbacks of g-C3N4,such as low surface area,poor diffusion,and charge separation efficiency,remain as the bottleneck to achieve highly efficient hydrogen evolution.Here,a hollow oxygen-incorporated g-C3N4 nanosheet(OCN)with an improved surface area of 148.5 m2 g^−1 is fabricated by the multiple thermal treatments under the N2/O2 atmosphere,wherein the C–O bonds are formed through two ways of physical adsorption and doping.The physical characterization and theoretical calculation indicate that the O-adsorption can promote the generation of defects,leading to the formation of hollow morphology,while the O-doping results in reduced band gap of g-C3N4.The optimized OCN shows an excellent photocatalytic hydrogen evolution activity of 3519.6μmol g^−1 h^−1 for~20 h,which is over four times higher than that of g-C3N4(850.1μmol g^−1 h^−1)and outperforms most of the reported g-C3N4 catalysts.

Nitrogen-doped Carbon Nanospheres-Modified Graphitic Carbon Nitride with Outstanding Photocatalytic Activity

Metals and metal oxides are widely used as photo/electro-catalysts for environmental remediation.However,there are many issues related to these metal-based catalysts for practical applications,such as high cost and detrimental environmental impact due to metal leaching.Carbon-based catalysts have the potential to overcome these limitations.In this study,monodisperse nitrogen-doped carbon nanospheres(NCs)were synthesized and loaded onto graphitic carbon nitride(g-C3N4,GCN)via a facile hydrothermal method for photocatalytic removal of sulfachloropyridazine(SCP).The prepared metal-free GCN-NC exhibited remarkably enhanced efficiency in SCP degradation.The nitrogen content in NC critically influences the physicochemical properties and performances of the resultant hybrids.The optimum nitrogen doping concentration was identified at 6.0 wt%.The SCP removal rates can be improved by a factor of 4.7 and 3.2,under UV and visible lights,by the GCN-NC composite due to the enhanced charge mobility and visible light harvesting.The mechanism of the improved photocatalytic performance and band structure alternation were further investigated by density functional theory(DFT)calculations.The DFT results confirm the high capability of the GCN-NC hybrids to activate the electron–hole pairs by reducing the band gap energy and efficiently separating electron/hole pairs.Superoxide and hydroxyl radicals are subsequently produced,leading to the efficient SCP removal.

Multidimensional(0D-3D)functional nanocarbon:Promising material to strengthen the photocatalytic activity of graphitic carbon nitride

As a prospective visible-light-responsive photochemical material,graphitic carbon nitride(g-C_(3)N_(4))has become a burgeoning research hot topics and aroused a wide interest as a metal-free semiconductor in the area of energy utilization and conversion,environmental protection due to its unique properties,such as facile synthesis,high physicochemical stability,excellent electronic band structure,and sustainability.However,the shortcomings of high recombination rate of charge carriers,relatively low electrical conductivity and visible light absorption impede its practical application.Various strategies,such as surface photosensitization,heteroatom deposition,semiconductor hybridization,etc.,have been applied to overcome the barriers.Among all the strategies,functional nanocarbon materials with various dimensions(0D~3D)attract much attention as modifiers of g-C_(3)N_(4)due to their unique electronic properties,optical properties,and easy functionalization.More importantly,the properties of these functional nanocarbon materials can be tuned by various dimensions and thus there will be a way to overcome the defects of g-C_(3)N_(4)by choosing different dimensional carbon materials.Distinguishing from some present reviews,this review starts with the fundamental physicochemical characteristics of g-C_(3)N_(4)materials,followed by analyzing the advantages of functional nanocarbon materials modifying gC_(3)N_(4).Then,we present a systematic introduction to various dimensional carbon materials.The design philosophy of carbon/g-C_(3)N_(4)composites and the advanced studies are exemplified in detail.Finally,a nichetargeting summary and outlook on the major challenges,opportunities for future research in high-powered carbon/g-C_(3)N_(4)composites was proposed.

Heteropolyacids-Immobilized Graphitic Carbon Nitride:Highly Efficient Photo-Oxidation of Benzyl Alcohol in the Aqueous Phase

Benzaldehyde is a highly desirable chemical due to its extensive application in medicine,chemical synthesis and food sector among others.However,its production generally involves hazardous solvents such as trifluorotoluene or acetonitrile,and its conversion,especially selectivity in the aqueous phase,is still not up to expectations.Hence,developing an environmentally benign,synthetic process for benzaldehyde production is of paramount importance.Herein,we report the preparation of a photocatalyst(PW_(12)-P-UCNS,where PW_(12)is H3PW_(12)O_(40)xH_(2)O and P-UCNS is phosphoric acid-modified unstack graphitic carbon nitride)by incorporating phosphotungstic acid on phosphoric acid-functionalised graphitic carbon nitride(g-C_(3)N_(4))nanosheets.The performance of PW_(12)-P-UCNS was tested using the benzyl alcohol photo-oxidation reaction to produce benzaldehyde in H_(2)O,at room temperature(20℃).The asprepared PW12-P-UCNS photocatalyst showed excellent photocatalytic performance with 58.3%conversion and 99.5%selectivity within 2 h.Moreover,the catalyst could be reused for at least five times without significant activity loss.Most importantly,a proposed Z-scheme mechanism of the PW_(12)-P-UCNScatalysed model reaction was revealed.We carefully investigated its transient photocurrent and electrochemical impedance,and identified superoxide radicals and photogenerated holes as the main active species through electron spin-resonance spectroscopy and scavenger experiments.Results show that the designed PW_(12)-P-UCNS photocatalyst is a highly promising candidate for benzaldehyde production through the photo-oxidation reaction in aqueous phase,under mild conditions.

Graphitic carbon nitride (g-C3N4)-based nanosized heteroarrays: Promising materials for photoelectrochemical water splitting

Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed.

Pomelo biochar as an electron acceptor to modify graphitic carbon nitride for boosting visible-light-driven photocatalytic degradation of tetracycline

In this study,biochar(BC)derived from pomelo was prepared via a high-temperature calcination method to modify the graphitic carbon nitride(g-C_(3)N_(4))to synthesize the BC/g-C_(3)N_(4)composite for the degradation of the tetracycline(TC)antibiotic under visible light irradiation.The experimental results exhibit that the optimal feeding weight ratio of biochar/urea is 0.03:1 in BC/g-C_(3)N_(4)composite could show the best photocatalytic activity with the degradation rate of tetracycline is 83%in 100 min irradiation.The improvement of photocatalytic activity is mainly attributed to the following two points:(i)the strong bonding with π-π stacking between BC and g-C_(3)N_(4)make the photogenerated electrons of light-excited g-C_(3)N_(4)transfer to BC,quickly and improve the separation efficiency of carriers;(ii)the introduction of BC reduces the distance for photogenerated electrons to migrate to the surface and increases the specific surface area for providing more active sites.This study provides a sustainable,economical and promising method for the synthesis of photocatalytic materials their application to wastewater treatment.

Three-dimensional graphitic carbon sphere foams as sorbents for cleaning oil spills

Frequent offshore oil spill accidents, industrial oily sewage, and the indiscriminate disposal of urban oily sewage have caused seri- ous impacts on the human living environment and health. The traditional oil-water separation methods not only cause easily environmental secondary pollution but also a waste of limited resources. Therefore, in this work, three-dimensional (3D) graphitic carbon sphere (GCS) foams (collectively referred hereafter as 3D foams) with a 3D porous structure, pore size distribution of 25-200 μm, and high porosity of 62vol% were prepared for oil adsorption via gel casting using GCS as the starting materials. The results indicate that the water contact angle (WCA) of the as-prepared 3D foams is 130°. The contents of GCS greatly influenced the hydrophobicity, WCA, and microstructure of the as-prepared samples. The adsorption capacities of the as-prepared 3D foams for paraffin oil, vegetable oil, and vacuum pump oil were approximately 12-15 g/g, which were 10 times that of GCS powder. The as-prepared foams are desirable characteristics of a good sorbent and could be widely used in oil spill accidents.

Tailoring structural properties of carbon via implanting optimal co nanoparticles in n-rich carbon cages toward high-efficiency oxygen electrocatalysis for rechargeable zn-air batteries

Rational construction of carbon-based materials with high-efficiency bifunctionality and low cost as the substitute of precious metal catalyst shows a highly practical value for rechargeable Zn-air batteries(ZABs)yet it still remains challenging.Herein,this study employs a simple mixing-calcination strategy to fabricate a high-performance bifunctional composite catalyst composed of N-doped graphitic carbon encapsulating Co nanoparticles(Co@NrC).Benefiting from the core-shell architectural and compositional advantages of favorable electronic configuration,more exposed active sites,sufficient electric conductivity,rich defects,and excellent charge transport,the optimal Co@NrC hybrid(Co@NrC-0.3)presents outstanding catalytic activity and stability toward oxygen-related electrochemical reactions(oxygen reduction and evolution reactions,i.e.,ORR and OER),with a low potential gap of 0.766 V.Besides,the rechargeable liquid ZAB assembled with this hybrid electrocatalyst delivers a high peak power density of 168 mW cm^(−2),a small initial discharge-charge potential gap of 0.45 V at 10 mA cm^(−2),and a good rate performance.Furthermore,a relatively large power density of 108 mW cm^(−2) is also obtained with the Co@NrC-0.3-based flexible solid-state ZAB,which can well power LED lights.Such work offers insights in developing excellent bifunctional electrocatalysts for both OER and ORR and highlights their potential applications in metal-air batteries and other energy-conversion/storage devices.