The potassium storage performance of carbon nanosheets derived from heavy oils

As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp3-C/sp2-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.

Flame-assisted ultrafast synthesis of functionalized carbon nanosheets for high-performance sodium storage

The unique structural features of hard carbon(HC)make it a promising anode candidate for sodium-ion batteries(SIB).However,traditional methods of preparing HC require special equipment,long reaction times,and large energy consumption,resulting in low throughputs and efficiency.In our contribution,a novel synthesis method is proposed,involving the formation of HC nanosheets(NS-CNs)within minutes by creating an anoxic environment through flame combustion and further introducing sulfur and nitrogen sources to achieve heteroatom doping.The effect of heterogeneous element doping on the microstructure of HC is quantitatively analyzed by high-resolution transmission electron microscopy and image processing technology.Combined with density functional theory calculation,it is verified that the functionalized HC exhibits stronger Na^(+)adsorption ability,electron gain ability,and Na^(+) migration ability.As a result,NS-CNs as SIB anodes provide an ultrahigh reversible capacity of 542.7mAh g^(-1) at 0.1Ag^(-1),and excellent rate performance with a reversible capacity of 236.4mAh g^(-1) at 2Ag^(-1) after 1200 cycles.Furthermore,full cell assembled with NS-CNs as the can present 230mAh g^(-1) at 0.5Ag^(-1) after 150 cycles.Finally,in/ex situ techniques confirm that the excellent sodium storage properties of NS-CNs are due to the construction of abundant active sites based on the novel synthesis method for realizing the reversible adsorption of Na^(+).This work provides a novel strategy to develop novel carbons and gives deep insights for the further investigation of facile preparation methods to develop high-performance carbon anodes for alkali-ion batteries.

Boosting the polysulfide confinement in B/N–codoped hierarchically porous carbon nanosheets via Lewis acid–base interaction for stable Li–S batteries

Carbon materials have shown remarkable usefulness in facilitating the performance of insulating sulfur cathode for lithium–sulfur batteries owing to their excellent conductivity and porous structure. However,the anxiety is the poor affinity toward polar polysulfides due to the intrinsic nonpolar surface of carbon.Herein, we report a direct pyrolysis of the mixture urea and boric acid to synthesize B/N–codoped hierarchically porous carbon nanosheets(B–N–CSs) as efficient sulfur host for lithium–sulfur battery. The graphene–like B–N–CSs provides high specific surface area and porous structure with abundant micropores(1.1 nm) and low–range mesopores(2.3 nm), thereby constraining the sulfur active materials within the pores. More importantly, the codoped B/N elements can further enhance the polysulfide confinement through strong Li–N and B–S interaction based on the Lewis acid–base theory. These structural superiorities significantly suppress the shuttle effect by both physical confinement and chemical interaction, and promote the redox kinetics of polysulfide conversion. When evaluated as the cathode host, the S/B–N–CSs composite displays the excellent performance with a high reversible capacity up to 772 m A h g–1 at 0.5 C and a low fading rate of ^0.09% per cycle averaged upon 500 cycles. In particular, remarkable stability with a high capacity retention of 87.1% can be realized when augmenting the sulfur loading in the cathode up to 4.6 mg cm^(-2).

Hierarchically porous, ultrathin N–doped carbon nanosheets embedded with highly dispersed cobalt nanoparticles as efficient sulfur host for stable lithium–sulfur batteries

The sluggish redox kinetics and shuttle effect of soluble polysulfides intermediate primarily restrict the electrochemical performance of lithium–sulfur(Li–S) batteries. To address this issue, rational design of high–efficiency sulfur host is increasingly demanded to accelerate the polysulfides conversion during charge/discharge process. Herein, we propose a macro–mesoporous sulfur host(Co@NC), which comprises highly dispersed cobalt nanoparticles embedding in N–doped ultrathin carbon nanosheets. Co@NC is simply synthesized via a carbon nitride–derived pyrolysis approach. Owing to the highly conductive graphene–like matrix and well defined porous structure, the designed multifunctional Co@NC host enables rapid electron/ion transport, electrolyte penetration and effective sulfur trapping. More significantly,N heteroatoms and homogeneous Co nanocatalysts in the graphitic carbon nanosheets could serve as chemisorption sites as well as electrocatalytic centers for sulfur species. These Co–N active sites can synergistically facilitate the redox conversion kinetics and mitigate the shuttling of polysulfides, thus leading to improved electrochemical cycling performance of Li–S batteries. As a consequence, the S/Co@NC cathode demonstrates high initial specific capacity(1505 mA h g-1 at 0.1 C) and excellent cycling stability at 1 C over 300 cycles, giving rise to a capacity retention of 91.7% and an average capacity decline of 0.03%cycle-1.

Micrometer-sized ferrosilicon composites wrapped with multi-layered carbon nanosheets as industrialized anodes for high energy lithium-ion batteries

Various nanostructured architectures have been demonstrated to be effective to address the issues of high capacity Si anodes. However, the scale-up of these nano-Si materials is still a critical obstacle for commercialization. Herein, we use industrial ferrosilicon as low-cost Si source and introduce a facile and scalable method to fabricate a micrometer-sized ferrosilicon/C composite anode, in which ferrosilicon microparticles are wrapped with multi-layered carbon nanosheets. The multi-layered carbon nanosheets could effectively buffer the volume variation of Si as well as create an abundant and reliable conductivity framework, ensuring fast transport of electrons. As a result, the micrometer-sized ferrosilicon/C anode achieves a stable cycling with 805.9 m Ah g-1 over 200 cycles at 500 mA g-1 and a good rate capability of455.6 mAh g-1 at 10 A g-1. Therefore, our approach based on ferrosilicon provides a new opportunity in fabricating cost-effective, pollution-free, and large-scale Si electrode materials for high energy lithium-ion batteries.

Carbon Nanosheets Encapsulated NiSb Nanoparticles as Advanced Anode Materials for Lithium-Ion Batteries

Metallic antimony(Sb) has been attracted much attentions as anode for lithium-ion batteries due to its high capacity.Nevertheless,the large volume expansion during the lithiation process leads to poor electrochemical performance,which seriously limits the practical application in lithium-ion batteries.Herein,NiSb nanoparticles encapsulated by carbon nanosheets have been developed via a facile strategy and as anode for lithium-ion batteries.In this attractive structure,the carbon nanosheets can effectively avoid volume change of NiSb nanoparticles and inhibit the direct contact of NiSb nanoparticles to the electrolyte during the lithiation/delithiation process.As a result,the NiSb/C nanosheets display an outstanding long cycling performance(405 mA h g-1 after 1000 cycles at 1.0 A g-1) and excellent rate capability(305 mA h g-1 at 2.0 A g-1) when application in lithium-ion batteries.

Cobalt-embedded few-layered carbon nanosheets toward enhanced hydrogen evolution:Rational design and insight into structure-performance correlation

Over the past decades, the energy and concomitant environment issues, such as energy shortage, air pollution and global warming, have been becoming increasingly striking world-wide challenges [1,2]. Such a dilemma in turn appeals to the development and employment of clean and renewable energy.

Binary molten salt in situ synthesis of sandwich-structure hybrids of hollowβ-Mo2C nanotubes and N-doped carbon nanosheets for hydrogen evolution reaction

Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water.Herein,a sandwich composite structure(designed as MS-Mo2C@NCNS)ofβ-Mo2C hollow nanotubes(HNT)and N-doped carbon nanosheets(NCNS)is designed and prepared using a binary NaCl–KCl molten salt(MS)strategy for HER.The temperature-dominant Kirkendall formation mechanism is tentatively proposed for such a three-dimensional hierarchical framework.Due to its attractive structure and componential synergism,MS-Mo2C@NCNS exposes more effective active sites,confers robust structural stability,and shows significant electrocatalytic activity/stability in HER,with a current density of 10 mA cm-2 and an overpotential of only 98 mV in 1 M KOH.Density functional theory calculations point to the synergistic effect of Mo2C HNT and NCNS,leading to enhanced electronic transport and suitable adsorption free energies of H*(ΔGH*)on the surface of electroactive Mo2C.More significantly,the MS-assisted synthetic methodology here provides an enormous perspective for the commercial development of highly active non-noble metal electrocatalysts toward efficient hydrogen evolution.

Controllable synthesis of grain boundary-enriched Pt nanoworms decorated on graphitic carbon nanosheets for ultrahigh methanol oxidation catalytic activity

Although one-dimensional Pt nanocrystals have long been regarded as ideal electrode catalysts for fuel cells,the synthetic techniques commonly involve the use of various complicated templates or surfactants,which have largely hampered their large-scale industrial application.Herein,we present a convenient and cost-effective approach to the stereoassembly of quasi-one-dimensional grain boundary-enriched Pt nanoworms on nitrogen-doped low-defect graphitic carbon nanosheets(Pt NWs/NL-CNS).Benefiting from its numerous catalytically active grain boundaries as well as optimized electronic structure,the as-derived Pt NWs/NL-CNS catalyst possesses exceptionally good electrocatalytic properties for methanol oxidation,including an ultrahigh mass activity of 1949.5 mA mg^(-1), reliable long-term durability,and strong poison tolerance,affording one of the most active Pt-based electrocatalysts for methanol oxidation reaction.Density functional theory calculation further reveals that the formation of worm-shape Pt morphology is attributed to the modified electronic structure as well as controllable defect density of the carbon matrix,which could also weaken the adsorption ability of Pt towards CO molecule and meanwhile synergistically promotes the catalytic reaction kinetics.

Co-Ru alloy nanoparticles decorated onto two-dimensional nitrogen doped carbon nanosheets towards hydrogen/oxygen evolution reaction and oxygen reduction reaction

Constructing highly-efficient electrocatalysts toward hydrogen evolution reaction(HER)/oxygen evolution reaction(OER)/oxygen reduction reaction(ORR)with excellent stability is quite important for the development of renewable energy-related applications.Herein,Co-Ru based compounds supported on nitrogen doped two-dimensional(2D)carbon nanosheets(NCN)are developed via one step pyrolysis procedure(Co-Ru/NCN)for HER/ORR and following low-temperature oxidation process(Co-Ru@RuO_(x)/NCN)for OER.The specific 2D morphology guarantees abundant active sites exposure.Furthermore,the synergistic effects arising from the interaction between Co and Ru are crucial in enhancing the catalytic performance.Thus,the resulting Co-Ru/NCN shows remarkable electrocatalytic performance for HER(70 mV at 10 mA cm^(-2))in 1 M KOH and ORR(half-wave potential E_(1/2)=0.81 V)in 0.1 M KOH.Especially,the Co-Ru@RuO_(x)/NCN obtained by oxidation exhibits splendid OER performance in both acid(230 mV at 10 mA cm^(-2))and alkaline media(270 mV at 10 mA cm^(-2))coupled with excellent stability.Consequently,the fabricated two-electrode water-splitting device exhibits excellent performance in both acidic and alkaline environments.This research provides a promising avenue for the advancement of multifunctional nanomaterials.

A Universal Strategy For N-Doped 2D Carbon Nanosheets With Sub-Nanometer Micropore For High-Performance Supercapacitor

Preparing carbon nanosheets with precise control of open porous morphology via universal process and understanding the relationship between structure and capacitive performance are very urgent for achieving advanced supercapacitors.Herein,we propose a simple yet effective additive-free method to transform a bulk layered potassium phthalimide salt to novel nitrogen-doped twodimensional carbon sheets by self-activation during calcination.The obtained samples showed large-sized and flat structure with lateral size around 10μm,uniform sub-nanometer micropore size distribution of about 0.65 nm dimension,large specific surface area up to 2276.7 m^(2)g^(-1),and suitable nitrogen doping.Benefited from these merits,the optimized sample delivers a high specific capacitance of 345 F g^(-1)at 1 A g^(-1)and retains 270 F g^(-1)even at 50 A g^(-1)in6.0 M KOH electrolyte.Remarkably,the symmetric supercapacitor shows maximum energy densities of 16.43 Wh kg^(-1)and 23.6 Wh kg^(-1)in 6.0 M KOH and 1.0 M Na_(2)SO_(4)electrolytes,respectively.Importantly,on account the universality and simplicity of this method,the undoped as-prepared carbon sheet with uniform sub-nanometer micropore distribution can be synthesized from different potassium-containing salts with layered structure,which can be employed as a model for a deep understanding the effect of sub-nanometer micropores on capacitive performances.We find the number of micropores centered at 0.65 nm can be applied as one indicator to clarify the correlation between capacitance and critical pore size below 1 nm.

High-temperature deoxygenation-created highly porous graphitic carbon nanosheets for ultrahigh-rate supercapacitive energy storage

Developing carbon-based supercapacitors with high rate capability is of great importance to meet the emerging demands for devices that requires high energy density as well as high power density.However,it is hard to fabricate a nanocarbon with high electro-active surface area meanwhile maintaining superior conductivity to ensure the high rate capability since excellent conductivity is usually realized by high temperature graphitization,which would lead to the structural collapse and sintering resulting in low surface area.Herein,we reported a highly porous graphitic carbon nanosheet with an unprecedented rate capability of 98%of its initial capacitance from 0.5 to 50 A/g for ultrahigh-rate supercapacitive energy storage.These hierarchical mesoporous carbon nanosheets(HMCN)were fabricated by a template induced catalytic graphitization approach,in which sheet-like Mg(OH)_(2) was employed as catalytic template in situ catalytically polymerizing of catechol and formaldehyde and catalytically graphitizing of the formed carbon skeleton.Upon the co-effect of template(avoiding the sintering)and the deoxygenation(creating the pores)during the high temperature graphitization process,the obtained HMCN material possesses nanosheet morphology with highly porous graphitic microstructure rich in mesoporosity,large in surface area(2316 m^(2)/g),large in pore volume(3.58 cm^(3)/g)and excellent in conductivity(109.8 S/cm).In 1.0 M TEABF_(4)/AN,HMCN exhibits superior supercapacitive performance including large energy density of 52.2 Wh/kg at high power density of 118 k W/kg,long-cycling stability and excellent rate capability,making HMCN a promising electrode material for supercapacitor devices.

CrN supported by carbon nanosheets as efficient catalysts toward oxygen reduction reaction and Zn-air batteries

Exploring non-precious efficient oxygen reduction reaction(ORR)catalysts is of great significance to fuel cells and Zn-air batteries(ZABs).CrN is a theoretically promising ORR catalyst,but its potential needs to be unlocked by proper supports that provide high conductivity and high exposure of active sites.In this work,we introduce a novel synthesis of carbon nanosheets-supported CrN nanoparticles(CrN/C)by annealing the mixture of CrCl_(3),1,10-phenanthroline and melamine via a two-step pyrolysis.The prepared CrN/C materials show good ORR activity and stability in acidic and alkaline media.The optimal CrN/C material has an ORR half-wave potential of 0.73 and 0.72 V(vs.reversible hydrogen electrode)in acidic and alkaline media,respectively.And it retains 82% and 78% of ORR current density in acidic and alkaline media after durability tests,respectively.Furthermore,the optimal CrN/C material-based self-breathing ZABs deliver a maximum power density of 168 mW·cm^(-2),which is one of the highest among transition metal nitrides-based ZABs It is found that the ORR activity of CrN/C materials is highly related to the Cr-N valence state.This work highlights the good potential of CrN as robust ORR catalyst and verifies its promising application in ZABs.

Stacking MoS_(2) flower-like microspheres on pomelo peels-derived porous carbon nanosheets for high-efficient X-band electromagnetic wave absorption

The key to solve increasingly severe electromagnetic(EM)pollution is to explore sustainable,easily prepared,and cost-effective EM wave absorption materials with exceptional absorption capability.Herein,instead of anchoring on carbon materials in single layer,MoS_(2) flower-like microspheres were stacked on the surface of pomelo peels-derived porous carbon nanosheets(C)to fabricate MoS_(2)@C nanocomposites by a facile solvothermal process.EM wave absorption performances of MoS_(2)@C nanocomposites in X-band were systematically investigated,indicating the minimum reflection loss(RLmin)of-62.3 dB(thickness of 2.88 mm)and effective absorption bandwidth(EAB)almost covering the whole X-band(thickness of 2.63 mm)with the filler loading of only 20 wt.%.Superior EM wave absorption performances of MoS_(2)@C nanocomposites could be attributed to the excellent impedance matching characteristic and dielectric loss capacity(conduction loss and polarization loss).This study revealed that the as-prepared MoS_(2)@C nanocomposites would be a novel prospective candidate for the sustainable EM absorbents with superior EM wave absorption performances.

Fe nanoclusters anchored in biomass waste-derived porous carbon nanosheets for high-performance supercapacitor

Metal-nanocluster materials have gradually become a promising electrode candidate for supercapaci-tor application.The high-efficient and rational architecture of these metal-nanocluster electrode mate-rials with satisfied supercapacitive performance are full of challenges.Herein,Fe-nanocluster anchored porous carbon(FAPC)nanosheets were constructed through a facile and low-cost impregnation-activation strategy.Various characterization methods documented that FAPC nanosheets possessed a mesopore-dominated structure with large surface area and abundant Fe-N4 active sites,which are crucial for su-percapacitive energy storage.The optimal FAPC electrode exhibited a high specific capacitance of 378 F/g at a specific current of 1 A/g and an excellent rate capability(271 F/g at 10 A/g),which are comparable or even superior to that of most reported carbon candidates.Furthermore,the FAPC-based device achieved a desired specific energy of 14.8 Wh/kg at a specific power of 700 W/kg.This work opens a new avenue to design metal-nanocluster materials for high-performance biomass waste-based supercapacitors.

Electrochemical Oxygen Evolution Performance of Nitrogen-Doped Ultra-Thin Carbon Nanosheets Composite Ru1Co Single Atom Alloy Catalysts

Energy transformation is imminent,and hydrogen energy is one of the important new energy sources.One of the keys to increasing the rate of hydrogen evolution during electrolysis is the use of high-performance catalysts for oxygen evolution reactions(OER).Single-atom alloys(SAAs)have garnered significant attention because they partially reduce costs and combine the advantages of both single-atom catalysts(SACs)and alloy catalysts.Herein,an efficient pyrolysis strategy based on a mixing and drying process is designed to anchor ultra-small Co cluster particles,combined with Ru single atoms dispersed on nitrogen-doped ultra-thin carbon nanosheets(Ru_(1)Co SAA/NC).The prepared electrocatalyst exhibits superior OER activity and superb stability,demonstrating an overpotential of 238 mV for OER with a current density of 10 mA·cm^(-2) in 0.5 mol/L H_(2)SO_(4).And we also utilized in-situ XAS to detect the oxidation state of Ru sites during OER.All in all,this method achieves cost reductions and efficiency improvements through the design of SAAs,offering new prospects for the structural transformation of clean energy.

FeNi Prussian blue analogues on highly graphitized carbon nanosheets as efficient glucose sensors

Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and stability.In this study,a straightforward strategy was proposed for synthesizing ultra-thin oxygen-rich graphitized carbon nanosheets(denoted as GCS-O).These nanosheets are obtained by calcining a topologically two-dimensional indium-based coordination polymer.Subsequently,the growth of FeNi Prussian blue analogue(PBA)on GCS-O effectively introduces active sites and increases the nitrogen content within the carbonaceous matrix.The resulting FeNi-PBA/GCS-O composite exhibits excellent glucose sensing performance with a broad linear range of 1 to 1300μmol·L^(-1).Meanwhile,it also achieves a high sensitivity of 2496μA·mmol^(-1)·L·cm^(-2),a limit of detection of 100nmol·L^(-1)(S/N=3),and commendable long-term durability.The relatively simple synthesis process,exceptional sensitivity,and satisfactory electrochemical sensing performance of FeNi-PBA/GCS-O open up new directions for biosensor applications.

Large-scale multirole Zn(Ⅱ) programmed synthesis of ultrathin hierarchically porous carbon nanosheets

ZIF-derived carbon structures are considered as desired electrode materials for supercapacitors due to their high surface area,high conductivity, and porous structure. However, the most reported ratio of 2-methylimidazole and Zn(II) is 4:1 to 20:1, which limits commercial applications due to the increasing cost. In this paper, a multirole Zn(II)-assisted method is presented from Zn(II) solution, Zn O, Zn O/ZIF-8 core-shell nanostructure, to 3 D hierarchical micro-meso-macroporous carbon structures with a1:1 ratio of 2-methylimidazole and Zn(II). The hierarchically porous carbon has a high surface area of 1800 m2 g^(-1) due to the synergistic effect of multirole Zn(II). The unique carbon-based half-cell delivers the specific capacitances of 377 and 221 F g^(-1) at the current densities of 1.0 and 50 A g^(-1), respectively. As a 2.5 V symmetrical supercapacitor, the device reveals a high doublelayer capacitance of 24.4 F g^(-1), a power density of 62.5 k W kg^(-1), and more than 85.8% capacitance can be retained over 10000 cycles at 10 A g^(-1). More importantly, the low-cost hierarchically porous carbon could be easily produced on a large scale and almost all chemicals can be reused in the sustainable method.

Multifunctional Templating Strategy for Fabrication of Fe,N-Codoped Hierarchical Porous Carbon Nanosheets

Due to the unique physical and chemical merits including excellent electrical conductivity,superior chemical stability,and tunable carbon framework,two-dimensional(2 D)porous carbon nanosheets have drawn increasing research interest and demonstrated promising potentials in various applications.However,regulating the nanostructure of 2 D porous carbon nanosheets by facile and efficient strategies remains a great challenge.Herein,we develop a new strategy to construct Fe,N-codoped hierarchical porous carbon nanosheets(Fe-N-HPCNS)by using 2 D Fe-Zn layered double hydroxides(Fe-Zn-LDH)as multifunctional templates.Fe-Zn-LDH could functionalize not only as 2 D structure directing agents but also as ternary hierarchical porogens for micro-,meso-and macropores and in situ Fe dopants.This multifunctional templating strategy toward 2 D porous carbon nanosheets can improve the utilization of templates and shows great advantages against conventional procedures that additional porogens and/or dopants are often needed.

In-situ Growth of Carbon Nanosheets Intercalated with TiO_(2) for Improving Electrochemical Performance and Stability of Lithium-ion Batteries

In situ growth of carbon nanomaterials on active substance is a very favorable strategy for the preparation of electrode in lithium-ion batteries with excellent electrochemical performance and high stability.Small-sized TiO_(2) nanoparticles intercalated into carbon nanosheets(CNS@TiO_(2)SNP-600)were successfully synthesized via in-situ polymerization-carbonization method,utilizing layered H_(2)Ti_(4)O_(9)(HTO)as template and benzidine as carbon source.The morphology and size of TiO_(2) are greatly influenced by carbonization temperature.The coin cell with the CNS@TiO_(2)SNP-600 electrode demonstrates a discharge specific capacity of 430.4 mAh·g^(-1) at a current density of 0.1 A·g^(-1),and the capacity retention rate is 88.1%after 100 cycles;and it also displays a high discharge specific capacity of 101.8 mAh·g^(-1) at a high current density of 12.8 A·g^(-1).The excellent electrochemical performances can be ascribed to the capacitance effect originated from the intercalated structure of in-situ grown CNS and TiO_(2) nanoparticles.We believe this type of materials can be widely used in the lithium-ion batteries and other related green chemical fields.