Organic-rich mudstones and shales,which hold significant potential for shale oil resources,characterize the first member of the Upper Cretaceous Qingshankou Formation(K_(2)qn~1)in the Sanzhao sag of the Songliao Basin...Organic-rich mudstones and shales,which hold significant potential for shale oil resources,characterize the first member of the Upper Cretaceous Qingshankou Formation(K_(2)qn~1)in the Sanzhao sag of the Songliao Basin,NE China.Focusing on 30 core samples obtained from the first shale oil parameter well,named SYY3 in the study area,we systematically analyzed the composition and stratigraphic distribution of the K_(2)qn~1 heteroatomic compounds using electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry(ESI FT-ICR MS),to assess their geological relevance to shale oil.The findings indicate that in the negative ion mode,the heteroatomic compounds predominantly consist of N_(1),N_(1)O_(1)-N_(1)O_(8),O_(1)-O_(8),O_(1)S_(1)-O_(6)S_(1);contrastingly,in the positive ion mode,they are primarily composed of N_(1)-N_(2),N_(1)O_(1)-N_(1)O_(4),N_(2)O_(1),O_(1)-O_(4),O_(1)S_(1)-O_(2)S_(1).Heteroatomic compound distributions vary significantly with depth in the negative ion mode,with minor variations in the positive ion mode.These distributions are categorized into three types based on the negative ion ratio((N_(1)+N_(1)O_(x))/O_(x)):TypeⅠ(>1.5),TypeⅡ(0.8-1.5),and TypeⅢ(<0.8);typesⅠandⅡgenerally exhibit a broader range of carbon numbers compared to TypeⅢ.The distribution of double bond equivalent(DBE)values across various sample types exhibits minimal variance,whereas that of carbon numbers shows substantial differences.Variations in heteroatomic compound compositions among the samples might have resulted from vertical sedimentary heterogeneity and differing biotic contributions.TypeⅢsamples show a decrease in total organic carbon(TOC)and free oil content(S_(1))compared to typesⅠandⅡ,but an increased oil saturation index(OSI),indicating a lower content of free oil but a higher proportion of movable oil.The reduced content of N-containing compounds implies lower paleolake productivity during deposition,leading to a reduction in TOC and S_(1).A lower TOC can enhance oil movability due to reduced oil adsorption,and the decreased presence of polar nitrogenous macromolecules with fewer highC-number heteroatomic compounds further promote shale oil movability.Additionally,the negative ion ratios of N1/N1O1and O2/O1 exhibit positive and negative correlations with the values of TOC,S_(1),and extractable organic matter(EOM),respectively,indicating that the salinity and redox conditions of the depositional water body are the primary controlling factors for both organic matter enrichment and shale oil accumulation.展开更多
The development of metal-free carbon catalysts has garnered significant attention as a promising approach to address the challenges of sustainable catalysis,particularly in the replacement of toxic and environmentally...The development of metal-free carbon catalysts has garnered significant attention as a promising approach to address the challenges of sustainable catalysis,particularly in the replacement of toxic and environmentally hazardous mercury-based systems for the coal-based PVC industry.Within a decade of development,the catalytic performance of carbon catalysts has been improved greatly and even shows superiorities over metal catalysts in some cases,which have demonstrated great potential as sustainable alternatives to mercury catalysts.This review provides a comprehensive summary of the recent advancements in carbon catalysts for acetylene hydrochlorination.It encompasses a wide range of aspects,including the identification of active sites from heteroatom doping to intrinsic carbon defects,the various synthetic strategies employed,the reaction and deactivation mechanisms of carbon catalysts,and the current insights into the key challenges that are encountered on the journey from laboratory research to scalable commercialization within the field of carbon catalysts.The review offers foundational insights and practical guidelines for designing green carbon catalysts systems,not only for acetylene hydrochlorination but also for other heterogeneous catalytic reactions.展开更多
Heavy oil,constituting a significant portion of global oil reserves,presents unique challenges in extraction and processing due to its high viscosity,largely influenced by asphaltenes and their heteroatom content.This...Heavy oil,constituting a significant portion of global oil reserves,presents unique challenges in extraction and processing due to its high viscosity,largely influenced by asphaltenes and their heteroatom content.This study employs molecular dynamics(MD)simulations to investigate the selfaggregation and adsorption mechanisms of heteroatom/non-heteroatom asphaltenes,comparing linear and island structural configurations.Key findings reveal that linear heteroatom asphaltenes form dense,multi-layered aggregates,while island heteroatom asphaltenes exhibit stronger aggregation energy.On solid surfaces,linear asphaltenes display multi-layered adsorption,whereas island asphaltenes adopt a dispersed structure with higher adsorption energy,making them more resistant to removal.Compared to non-heteroatom asphaltenes,heteroatom asphaltenes significantly enhance the aggregation energy of the asphaltene itself and the interaction energy with light oil components,reducing the diffusion capacity of oil droplets and increasing viscosity.Although the viscosity of island heteroatom asphaltene oil drops is the largest,the role of heteroatom in linear asphaltene is more obvious,and linear heteroatom asphaltene and non-heteroatom show great differences in properties.Additionally,heteroatom-containing oil droplets exhibit stronger interactions with solid surfaces,driven by the influence of heteroatom asphaltenes on lighter oil components.These insights provide a deeper understanding of heavy oil viscosity mechanisms,offering a foundation for developing targeted viscosity-reduction strategies and optimizing heavy oil recovery and processing techniques.展开更多
Electrocatalyst activity and stability demonstrate a“seesaw”relationship.Introducing vacancies(Vo)enhances the activity by improving reactant affinity and increasing accessible active sites.However,deficient or exce...Electrocatalyst activity and stability demonstrate a“seesaw”relationship.Introducing vacancies(Vo)enhances the activity by improving reactant affinity and increasing accessible active sites.However,deficient or excessive Vo reduces polysulfide adsorption and lowers catalytic stability.Herein,a novel“heteroatoms synergistic anchoring vacancies”strategy is proposed to address the trade-off between high activity and stability.Phosphorus-doped CoSe_(2)with remained rich selenium vacancies(P-CS-Vo-0.5)was synthesized by producing abundant selenium Vo followed by controlled P atom doping.Atomic-scale microstructure analysis elucidated a dynamic process of surface vacancy generation and the subsequent partial occupation of these vacancies by P atoms.Density functional theory simulations and in situ Raman tests revealed that the Se vacancies provide highly active catalytic sites,accelerating polysulfide conversion,while P incorporation effectively reduces the surface energy of Se vacancies and suppresses their inward migration,enhancing structural robustness.The battery with the optimal P-CS-Vo-0.5 separator delivers an initial discharge capacity of 1306.7 mAh g^(-1)at 0.2C,and maintain 5.04 mAh cm^(-2)at a high sulfur loading(5.7 mg cm^(-2),5.0μL mg^(-1)),achieving 95.1%capacity retention after 80 cycles.This strategy of modifying local atomic environments offers a new route to designing highly active and stable catalysts.展开更多
The Ni single-atom catalyst dispersed on nitrogen doped graphene support has attracted much interest due to the high selectivity in electro-catalyzing CO_(2)reduction to CO,yet the chemical inertness of the metal cent...The Ni single-atom catalyst dispersed on nitrogen doped graphene support has attracted much interest due to the high selectivity in electro-catalyzing CO_(2)reduction to CO,yet the chemical inertness of the metal center renders it to exhibit electrochemical activity only under high overpotentials.Herein,we report P-and S-doped Ni single-atom catalysts,i.e.symmetric Ni_(1)/PN_(4)and asymmetric Ni1/SN_(3)C can exhibit high catalytic activity of CO_(2)reduction with stable potential windows.It is revealed that the key intermediate*COOH in CO_(2)electroreduction is stabilized by heteroatom doping,which stems from the upward shift of the axial d_(z2)orbital of the active metal Ni atom.Furthermore,we investigate the potential-dependent free energetics and dynamic properties at the electrochemical interface on the Ni1/SN3C catalyst using ab initio molecular dynamics simulations with a full explicit solvent model.Based on the potential-dependent microkinetic model,we predict that S-atom doped Ni SAC shifts the onset potential of CO_(2)electroreduction from–0.88 to–0.80 V vs.RHE,exhibiting better activity.Overall,this work provides an in-depth understanding of structure-activity relationships and atomic-level electrochemical interfaces of catalytic systems,and offers insights into the rational design of heteroatom-doped catalysts for targeted catalysis.展开更多
Lithium-sulfur batteries(LSBs)have received much concern as emerging high-power energy storage system.Nevertheless,the low conductivity of sulfur and poly sulfide shuttle results in low rate capability and rapid capac...Lithium-sulfur batteries(LSBs)have received much concern as emerging high-power energy storage system.Nevertheless,the low conductivity of sulfur and poly sulfide shuttle results in low rate capability and rapid capacity decay,which seriously limit its commercial application.Here,facile,sustainable and cost-effective strategy for preparing heteroatom-doped porous activated carbon(PAC)derived from biomass palm kernel shell(PKS)was developed for high-performance LSB applications.The presence of N,P and S heteroatoms with modification of the surface polarity brings about large amounts of active sites and improved adsorption property compared to those of common carbon materials.The PAC sample possesses desirable specific surface area(SSA)(2760 m2·g-1)as well as pore volume(1.6 cm3·g-1).Besides,the good electrical conductivity of PAC endows the material with excellent rate performance.The PAC-S electrode with a 60%of sulfur loading has a desirable first discharge capacity(1045 mAh·g1,200 mA·g-1)with superb discharge capacity(869.8 mAh·g-1,100 th cycle)and cyclability(312.6 mAh·g-1,800 mA·g-1,1000 th cycle),which can be mainly ascribed to its unique porous properties and the good conductivity of PAC.展开更多
Incorporation of heteroatoms into the framewo rk of zeolites has become a significant strategy to improve their performance in catalysis and adsorption,because the obtained heteroatom zeolites exhibit quite different ...Incorporation of heteroatoms into the framewo rk of zeolites has become a significant strategy to improve their performance in catalysis and adsorption,because the obtained heteroatom zeolites exhibit quite different properties from the conventional aluminosilicate zeolites in aspects of surface acidity,pore structures,particle size and so on.In this review,the progress on the heteroatom zeolites including their synthesis and application is highlighted.First,the recent advance on the design and synthesis of different heteroatom zeolites is summarized.Special emphasis is placed on the introduction and comparison of three typical methods,including the direct synthesis,post synthesis and improved direct synthesis,for the traditional heteroatom zeolites(such as TS-1,Sn-MFI,Sn-β) and newly-reported heteroatom zeolites(such as W-MFI,Mo-MFI).According to their intrinsic characteristics,the application of heteroatom zeolites in diverse fields,such as production of fine chemicals,air pollution control and biomass conversion is then discussed.Finally,the challenges and perspective on the future development of heteroatom zeolites in low-cost preparation and practical application are proposed.展开更多
Rhodamine is one class of most popular dyes used in fluorescence imaging due to the outstanding photoproperties including high brightness and photostability. In recent years, replacement the xanthene oxygen with other...Rhodamine is one class of most popular dyes used in fluorescence imaging due to the outstanding photoproperties including high brightness and photostability. In recent years, replacement the xanthene oxygen with other elements, especially silicon, has attracted great attentions in the development of new rhodamine derivatives. This review summarized the structures and photophysical properties of heteroatom-substituted rhodamines. We hope this review can help to understand the structure-property relationships of rhodamine dyes and then elucidate the way to create derivatives with improved photoproperties.展开更多
The large-scale application of sodium ion batteries(SIBs)is limited by economic and environmental factors.Here,we prepare multi-heteroatom self-doped hierarchical porous carbon(HHPC)with a honeycomb-like structure by ...The large-scale application of sodium ion batteries(SIBs)is limited by economic and environmental factors.Here,we prepare multi-heteroatom self-doped hierarchical porous carbon(HHPC)with a honeycomb-like structure by one-step carbonization method using high-yield and low-cost biomass silkworm excrement as a precursor.As an anode for SIB,HHPC-1100 exhibits a capacity of 331.7 mA h g^(-1) at 20 mA g^(-1),while it also reveals remarkable rate performance and stable long cycle capability due to its abundant pore structure and proper amount of hetero atom doping.Moreover,the synergistic effect of O,N,S,P co-doping in carbon materials on sodium ion adsorption is verified by the first-principles study,which provide a theoretical basis for the prominent electrochemical performance of the material.展开更多
Banana peel-derived porous carbon(BPPC) was prepared from banana peel and used as an adsorbent for methyl orange(MO) wastewater removal. BPPC-MO50 is a N,S-doped BPPC obtained via secondary carbonization. The BPPC-MO5...Banana peel-derived porous carbon(BPPC) was prepared from banana peel and used as an adsorbent for methyl orange(MO) wastewater removal. BPPC-MO50 is a N,S-doped BPPC obtained via secondary carbonization. The BPPC-MO50 exhibited a high specific surface area of1774.3 m^2/g. Heteroatom-doped porous carbon(PC) was successfully synthesized from the BPPC absorbed MO at high temperature and used for oxygen reduction. The BPPC-MO50 displayed the highest ORR onset potential among all carbon-based electrocatalysts, i.e., 0.93 V vs.reversible hydrogen electrode(RHE). This is the first report to describe porous carbon-activated materials from agriculture and forestry waste that is used for adsorption of dyes from wastewater via an enhanced heteroatom(N,S) content. These results may contribute to the sustainable development of dye wastewater treatment by transforming saturated PC into an effective material and has potential applications in fuel cells or as energy sources.展开更多
Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Hetero...Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Heteroatom modification is one of the most effective strategies for boosting catalytic performance,as it can regulate the physicochemical properties of host catalysts to improve their intrinsic activity.Herein,aiming to provide an overview of the impact of heteroatoms on catalytic activity at the atomic level,we present a review of the key role of heteroatoms in enhancing reaction kinetics based on the reaction pathways of the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline media.In particular,the introduction of heteroatoms can directly and indirectly optimize the interactions between the active sites and intermediates,thus improving the intrinsic activity.To clearly illustrate this influence in detail,we have summarized a series of representative heteroatom-modified electrocatalysts and discussed the important roles of heteroatoms in the OER and HER reaction pathways.Finally,some challenges and perspectives for heteroatom-modified electrodes are discussed.We hope that this review will be helpful for the development of efficient and low-cost electrocatalysts for water electrolysis and other energy conversion applications.展开更多
Hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen ...Hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen evolution reaction(HER)/hydrazine oxidation reaction(HzOR)kinetics,is the key step.Herein,we demonstrate the development of ultrathin P/Fe co-doped NiSe_(2) nanosheets supported on modified Ni foam(P/Fe-NiSe_(2)) synthesized through a facile electrodeposition process and subsequent heat treatment.Based on electrochemical measurements,characterizations,and density functional theory calculations,a favorable“2+2”reaction mechanism with a two-step HER process and a two-step HzOR step was fully proved and the specific effect of P doping on HzOR kinetics was investigated.P/Fe-NiSe_(2) thus yields an impressive electrocatalytic performance,delivering a high current density of 100 mA cm^(−2) with potentials of−168 and 200 mV for HER and HzOR,respectively.Additionally,P/Fe-NiSe_(2) can work efficiently for hydrazine-assisted water electrolysis and Zn-Hydrazine(Zn-Hz)battery,making it promising for practical application.展开更多
Delafossite CuFeO_(2) is a promising photocathode material for cost-efficiently photoelectrochemical(PEC)water splitting,but the unfavorable conductivity and fast recombination dynamics of photogenerated carriers limi...Delafossite CuFeO_(2) is a promising photocathode material for cost-efficiently photoelectrochemical(PEC)water splitting,but the unfavorable conductivity and fast recombination dynamics of photogenerated carriers limit its PEC activity for water reduction.Here,we developed a heterostructure photocathode consisting of the Cu-doped NiO(Cu:NiO)hole selective layer(HSL)and Ni-doped CuFeO_(2)(Ni:CuFeO_(2))active layer by simply annealing a homogeneous Cu-Fe oxalate layer grown on the Ni film deposited on the fluorine doped tin oxide(FTO)substrate.The obtained heterostructure of Cu:NiO/Ni:CuFeO_(2) with enhanced charge carrier transportability and high-quality interface greatly promotes the separation of photogenerated carriers.Accordingly,the Cu:NiO/Ni:CuFeO_(2) photocathode exhibits a high photocurrent density of~0.9 mA·cm^(-2 )at 0.2 V(vs.reversible hydrogen electrode,RHE),outperforming most of the reported bare CuFeO_(2) photocathodes in the literature.And the photocurrent density can be further improved to 1.2 mA·cm^(-2) after decorating NiSx cocatalyst.展开更多
A new rhodium catalyzed ring opening reaction of oxabenzonorbornadienes and its derivatives was described. This reaction forms a new carbon-nitrogen bond via an intermolecular allylic displacement of the bridgehead o...A new rhodium catalyzed ring opening reaction of oxabenzonorbornadienes and its derivatives was described. This reaction forms a new carbon-nitrogen bond via an intermolecular allylic displacement of the bridgehead oxygen with a piperazine's derivatives, which proceeds with very high regioselectivity.展开更多
CeO2,Ce1–xZrxO2,and Ce1–xYxO2–δ(x=0.25,0.50,0.75,and 1.00)have been rapidly synthesized to estimate their catalytic behavior in decomposing CH3SH.The role of oxygen vacancies,and the relationship between the oxyge...CeO2,Ce1–xZrxO2,and Ce1–xYxO2–δ(x=0.25,0.50,0.75,and 1.00)have been rapidly synthesized to estimate their catalytic behavior in decomposing CH3SH.The role of oxygen vacancies,and the relationship between the oxygen species and catalytic properties of CeO2 and Zr‐doped and Y‐doped ceria‐based materials are investigated in detail.Combining the observed catalytic performance with the characterization results,it can be deemed that surface lattice oxygen plays a critical role in methanethiol catalytic conversion over cerium oxides.Ce0.75Zr0.25O2 shows higher catalytic activity for CH3SH decomposition due to the large amount of surface lattice oxygen,readily available oxygen species,and excellent redox properties.Ce0.75Y0.25O2–δdisplays better catalytic stability owing to the greater number of oxygen vacancies that would promote bulk lattice oxygen migration to the surface of the catalyst in order to replenish surface lattice oxygen.In addition,the results show that the difference in chemical valence between Ce and the heteroatoms would strongly influence the amount of surface lattice oxygen as well as the mobility of bulk‐phase oxygen in these catalysts,thus affecting their activity and stability.展开更多
Research on asymmetric A–D–A structured non-fullerene acceptors has lagged far behind the development of symmetric counterpart.In this contribution,by simply replacing one sulfur atom in indacenodithiophene unit wit...Research on asymmetric A–D–A structured non-fullerene acceptors has lagged far behind the development of symmetric counterpart.In this contribution,by simply replacing one sulfur atom in indacenodithiophene unit with a selenium atom,an asymmetric building block Se PT and a corresponding asymmetric non-fullerene acceptor Se PT-IN have been developed.Asymmetric Se PT-IN achieved a high efficiency of 10.20% in organic solar cells when blended with PBT1-C,much higher than that of symmetric TPT-IN counterpart(8.91%).Our results demonstrated an effective heteroatom substitution strategy to develop asymmetric A–D–A structured non-fullerene acceptors.展开更多
Activated carbons for electrochemical capacitor electrodes are prepared from soyabean using chemical activation with KOH. The pore size is easily controllable by changing the mass ratio between KOH and carbonized prod...Activated carbons for electrochemical capacitor electrodes are prepared from soyabean using chemical activation with KOH. The pore size is easily controllable by changing the mass ratio between KOH and carbonized product. The as-prepared materials possess a large specific surface area, unique structure, well- developed hierarchical porosity and plentiful heteroatoms（mainly O and N）. Thus resulted in its high specific capacitance,good rate capacity and cycling stability. Moreover, attributing to worldwide availability, renewable nature and low-cost, activated carbon prepared from soyabean has a good potential in energy conversion and storage devices.展开更多
Carbon dioxide(CO_(2))reduction into chemicals or fuels by electrocatalysis can eff ectively reduce greenhouse gas emissions and alleviate the energy crisis.Currently,CO_(2)electrocatalytic reduction(CO_(2)RR)has been...Carbon dioxide(CO_(2))reduction into chemicals or fuels by electrocatalysis can eff ectively reduce greenhouse gas emissions and alleviate the energy crisis.Currently,CO_(2)electrocatalytic reduction(CO_(2)RR)has been considered as an ideal way to achieve“carbon neutrality.”In CO_(2)RR,the characteristics and properties of catalysts directly determine the reaction activity and selectivity of the catalytic process.Much attention has been paid to carbon-based catalysts because of their diversity,low cost,high availability,and high throughput.However,electrically neutral carbon atoms have no catalytic activity.Incorpo-rating heteroatoms has become an eff ective strategy to control the catalytic activity of carbon-based materials.The doped carbon-based catalysts reported at present show excellent catalytic performance and application potential in CO_(2)RR.Based on the type and quantity of heteroatoms doped into carbon-based catalysts,this review summarizes the performances and catalytic mechanisms of carbon-based materials doped with a single atom(including metal and without metal)and multi atoms(including metal and without metal)in CO_(2)RR and reveals prospects for developing CO_(2)electroreduction in the future.展开更多
Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons...Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities.Nevertheless,most lignocellulose biomasses lack heteroatoms,making it a challenge to design highly heteroatom-doped carbons(>10 at%).Herein,we report a new preparation strategy for amorphous carbon anodes.Nitrogen/sulfur co-doped lignin-derived porous carbons(NSLPC)with ultra-high nitrogen doping levels(21.6 at%of N and 0.8 at%of S)from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy.This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product,which induces the formation of high heteroatom doping in the obtained NSLPC.This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K+and improved kinetics.The NSLPC anode delivered a high reversible capacity of 419 mAh g^(-1)and superior cycling stability(capacity retention of 96.6%at 1 A g^(-1)for 1000 cycles).Potassiumion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability(91%capacity retention for 2000 cycles)and a high energy density of 71 Wh kg^(-1)at a power density of 92 W kg^(-1).展开更多
Non-graphitized carbon(NGC)has been extensively utilized as carbonaceous anode in sodium-ion batteries(SIBs).However,more optimization to achieve competitive capacity and stability is still challenging for SIBs.In the...Non-graphitized carbon(NGC)has been extensively utilized as carbonaceous anode in sodium-ion batteries(SIBs).However,more optimization to achieve competitive capacity and stability is still challenging for SIBs.In the study,the dopant strategy is utilized to construct nitrogen/sulfur-doped non-graphitized carbon(N-NGC or S-NGC)shell decorated on three-dimensional graphene foam(GF)as a self-support electrode.The highly disordered microstructures of heteroatom doped carbons are produced by applying a low-temperature pyrolysis treatment to precursors containing nitrogen and sulfur.The DFT calculations of Na-ion adsorption energies at diverse heteroatom sites show marginal-S,pyrrolic N and pyridinic N with more intensive Na-ion adsorption ability than middle-S,C=O and pristine carbon.The N-NGC with dominant small graphitic regions delivers adsorption ability to Na-ion,while the S-NGC with significant single carbon lattice stripes demonstrates redox reaction with Na-ion.Evidently,in comparison with only adsorption-driven slope regions at high potential for N-NGC,the redox reaction-generated potentialplateau enables non-graphitized S-NGC superior discharge/charge capacity and cycle-stability in the slope region.This work could provide deep insight into the rational design of non-graphitized carbon with rich microstructure and composition.展开更多
基金jointly funded by the National Natural Science Foundation of China(Grant Nos.42072178 and U2244207)the funding project of Northeast Geological S&T Innovation Center of China Geological Survey(Grant No.QCJJ2022-37)Geological Survey Project of China Geological Survey(Grant Nos.DD20190114,DD20230022,and DD20240045)。
文摘Organic-rich mudstones and shales,which hold significant potential for shale oil resources,characterize the first member of the Upper Cretaceous Qingshankou Formation(K_(2)qn~1)in the Sanzhao sag of the Songliao Basin,NE China.Focusing on 30 core samples obtained from the first shale oil parameter well,named SYY3 in the study area,we systematically analyzed the composition and stratigraphic distribution of the K_(2)qn~1 heteroatomic compounds using electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry(ESI FT-ICR MS),to assess their geological relevance to shale oil.The findings indicate that in the negative ion mode,the heteroatomic compounds predominantly consist of N_(1),N_(1)O_(1)-N_(1)O_(8),O_(1)-O_(8),O_(1)S_(1)-O_(6)S_(1);contrastingly,in the positive ion mode,they are primarily composed of N_(1)-N_(2),N_(1)O_(1)-N_(1)O_(4),N_(2)O_(1),O_(1)-O_(4),O_(1)S_(1)-O_(2)S_(1).Heteroatomic compound distributions vary significantly with depth in the negative ion mode,with minor variations in the positive ion mode.These distributions are categorized into three types based on the negative ion ratio((N_(1)+N_(1)O_(x))/O_(x)):TypeⅠ(>1.5),TypeⅡ(0.8-1.5),and TypeⅢ(<0.8);typesⅠandⅡgenerally exhibit a broader range of carbon numbers compared to TypeⅢ.The distribution of double bond equivalent(DBE)values across various sample types exhibits minimal variance,whereas that of carbon numbers shows substantial differences.Variations in heteroatomic compound compositions among the samples might have resulted from vertical sedimentary heterogeneity and differing biotic contributions.TypeⅢsamples show a decrease in total organic carbon(TOC)and free oil content(S_(1))compared to typesⅠandⅡ,but an increased oil saturation index(OSI),indicating a lower content of free oil but a higher proportion of movable oil.The reduced content of N-containing compounds implies lower paleolake productivity during deposition,leading to a reduction in TOC and S_(1).A lower TOC can enhance oil movability due to reduced oil adsorption,and the decreased presence of polar nitrogenous macromolecules with fewer highC-number heteroatomic compounds further promote shale oil movability.Additionally,the negative ion ratios of N1/N1O1and O2/O1 exhibit positive and negative correlations with the values of TOC,S_(1),and extractable organic matter(EOM),respectively,indicating that the salinity and redox conditions of the depositional water body are the primary controlling factors for both organic matter enrichment and shale oil accumulation.
文摘The development of metal-free carbon catalysts has garnered significant attention as a promising approach to address the challenges of sustainable catalysis,particularly in the replacement of toxic and environmentally hazardous mercury-based systems for the coal-based PVC industry.Within a decade of development,the catalytic performance of carbon catalysts has been improved greatly and even shows superiorities over metal catalysts in some cases,which have demonstrated great potential as sustainable alternatives to mercury catalysts.This review provides a comprehensive summary of the recent advancements in carbon catalysts for acetylene hydrochlorination.It encompasses a wide range of aspects,including the identification of active sites from heteroatom doping to intrinsic carbon defects,the various synthetic strategies employed,the reaction and deactivation mechanisms of carbon catalysts,and the current insights into the key challenges that are encountered on the journey from laboratory research to scalable commercialization within the field of carbon catalysts.The review offers foundational insights and practical guidelines for designing green carbon catalysts systems,not only for acetylene hydrochlorination but also for other heterogeneous catalytic reactions.
基金supported financially by the National Natural Science Foundation of China(No.52204069,No.22306171)the Natural Science Foundation of Zhejiang Province(No.LQ24B070005)the Jinhua Natural Science Foundation of China(2023-4-024)。
文摘Heavy oil,constituting a significant portion of global oil reserves,presents unique challenges in extraction and processing due to its high viscosity,largely influenced by asphaltenes and their heteroatom content.This study employs molecular dynamics(MD)simulations to investigate the selfaggregation and adsorption mechanisms of heteroatom/non-heteroatom asphaltenes,comparing linear and island structural configurations.Key findings reveal that linear heteroatom asphaltenes form dense,multi-layered aggregates,while island heteroatom asphaltenes exhibit stronger aggregation energy.On solid surfaces,linear asphaltenes display multi-layered adsorption,whereas island asphaltenes adopt a dispersed structure with higher adsorption energy,making them more resistant to removal.Compared to non-heteroatom asphaltenes,heteroatom asphaltenes significantly enhance the aggregation energy of the asphaltene itself and the interaction energy with light oil components,reducing the diffusion capacity of oil droplets and increasing viscosity.Although the viscosity of island heteroatom asphaltene oil drops is the largest,the role of heteroatom in linear asphaltene is more obvious,and linear heteroatom asphaltene and non-heteroatom show great differences in properties.Additionally,heteroatom-containing oil droplets exhibit stronger interactions with solid surfaces,driven by the influence of heteroatom asphaltenes on lighter oil components.These insights provide a deeper understanding of heavy oil viscosity mechanisms,offering a foundation for developing targeted viscosity-reduction strategies and optimizing heavy oil recovery and processing techniques.
基金supported by the National Key Research and Development Program of China(No.2022YFA1602700 and 2022YFB2502104)the National Natural Science Foundation of China(22375089)the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology of China(BE2022332).
文摘Electrocatalyst activity and stability demonstrate a“seesaw”relationship.Introducing vacancies(Vo)enhances the activity by improving reactant affinity and increasing accessible active sites.However,deficient or excessive Vo reduces polysulfide adsorption and lowers catalytic stability.Herein,a novel“heteroatoms synergistic anchoring vacancies”strategy is proposed to address the trade-off between high activity and stability.Phosphorus-doped CoSe_(2)with remained rich selenium vacancies(P-CS-Vo-0.5)was synthesized by producing abundant selenium Vo followed by controlled P atom doping.Atomic-scale microstructure analysis elucidated a dynamic process of surface vacancy generation and the subsequent partial occupation of these vacancies by P atoms.Density functional theory simulations and in situ Raman tests revealed that the Se vacancies provide highly active catalytic sites,accelerating polysulfide conversion,while P incorporation effectively reduces the surface energy of Se vacancies and suppresses their inward migration,enhancing structural robustness.The battery with the optimal P-CS-Vo-0.5 separator delivers an initial discharge capacity of 1306.7 mAh g^(-1)at 0.2C,and maintain 5.04 mAh cm^(-2)at a high sulfur loading(5.7 mg cm^(-2),5.0μL mg^(-1)),achieving 95.1%capacity retention after 80 cycles.This strategy of modifying local atomic environments offers a new route to designing highly active and stable catalysts.
文摘The Ni single-atom catalyst dispersed on nitrogen doped graphene support has attracted much interest due to the high selectivity in electro-catalyzing CO_(2)reduction to CO,yet the chemical inertness of the metal center renders it to exhibit electrochemical activity only under high overpotentials.Herein,we report P-and S-doped Ni single-atom catalysts,i.e.symmetric Ni_(1)/PN_(4)and asymmetric Ni1/SN_(3)C can exhibit high catalytic activity of CO_(2)reduction with stable potential windows.It is revealed that the key intermediate*COOH in CO_(2)electroreduction is stabilized by heteroatom doping,which stems from the upward shift of the axial d_(z2)orbital of the active metal Ni atom.Furthermore,we investigate the potential-dependent free energetics and dynamic properties at the electrochemical interface on the Ni1/SN3C catalyst using ab initio molecular dynamics simulations with a full explicit solvent model.Based on the potential-dependent microkinetic model,we predict that S-atom doped Ni SAC shifts the onset potential of CO_(2)electroreduction from–0.88 to–0.80 V vs.RHE,exhibiting better activity.Overall,this work provides an in-depth understanding of structure-activity relationships and atomic-level electrochemical interfaces of catalytic systems,and offers insights into the rational design of heteroatom-doped catalysts for targeted catalysis.
基金financially supported by the National Natural Science Foundation of China(Nos.21671170,21673203,21805136 and 21201010)the Natural Science Foundation of Jiangsu Province(No.BK20170999)+2 种基金Program for New Century Excellent Talents of the University in China(No.NCET-13-0645)the Six Talent Plan(No.2015-XCL-030)Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘Lithium-sulfur batteries(LSBs)have received much concern as emerging high-power energy storage system.Nevertheless,the low conductivity of sulfur and poly sulfide shuttle results in low rate capability and rapid capacity decay,which seriously limit its commercial application.Here,facile,sustainable and cost-effective strategy for preparing heteroatom-doped porous activated carbon(PAC)derived from biomass palm kernel shell(PKS)was developed for high-performance LSB applications.The presence of N,P and S heteroatoms with modification of the surface polarity brings about large amounts of active sites and improved adsorption property compared to those of common carbon materials.The PAC sample possesses desirable specific surface area(SSA)(2760 m2·g-1)as well as pore volume(1.6 cm3·g-1).Besides,the good electrical conductivity of PAC endows the material with excellent rate performance.The PAC-S electrode with a 60%of sulfur loading has a desirable first discharge capacity(1045 mAh·g1,200 mA·g-1)with superb discharge capacity(869.8 mAh·g-1,100 th cycle)and cyclability(312.6 mAh·g-1,800 mA·g-1,1000 th cycle),which can be mainly ascribed to its unique porous properties and the good conductivity of PAC.
基金supported by the National Natural Science Foundation of China(Nos.21875044,21673048)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.17JC1400100)+2 种基金the support by the state key laboratory of Transducer Technology of China(No.SKT1904)Program of Shanghai Academic Research Leader(No.19XD1420300)Research Supporting Project(No.RSP-2019/155)by King Saud University。
文摘Incorporation of heteroatoms into the framewo rk of zeolites has become a significant strategy to improve their performance in catalysis and adsorption,because the obtained heteroatom zeolites exhibit quite different properties from the conventional aluminosilicate zeolites in aspects of surface acidity,pore structures,particle size and so on.In this review,the progress on the heteroatom zeolites including their synthesis and application is highlighted.First,the recent advance on the design and synthesis of different heteroatom zeolites is summarized.Special emphasis is placed on the introduction and comparison of three typical methods,including the direct synthesis,post synthesis and improved direct synthesis,for the traditional heteroatom zeolites(such as TS-1,Sn-MFI,Sn-β) and newly-reported heteroatom zeolites(such as W-MFI,Mo-MFI).According to their intrinsic characteristics,the application of heteroatom zeolites in diverse fields,such as production of fine chemicals,air pollution control and biomass conversion is then discussed.Finally,the challenges and perspective on the future development of heteroatom zeolites in low-cost preparation and practical application are proposed.
基金financially supported by the National Natural Science Foundation China (No. 21878286)DICP (Nos. DMTO201603, TMSR201601)
文摘Rhodamine is one class of most popular dyes used in fluorescence imaging due to the outstanding photoproperties including high brightness and photostability. In recent years, replacement the xanthene oxygen with other elements, especially silicon, has attracted great attentions in the development of new rhodamine derivatives. This review summarized the structures and photophysical properties of heteroatom-substituted rhodamines. We hope this review can help to understand the structure-property relationships of rhodamine dyes and then elucidate the way to create derivatives with improved photoproperties.
基金supported by the National Natural Science Foundation of China(Grant No.51872236)the Joint Fund ProjectEnterprise-Shaanxi Coal Joint Fund Project(2019JLM-32)。
文摘The large-scale application of sodium ion batteries(SIBs)is limited by economic and environmental factors.Here,we prepare multi-heteroatom self-doped hierarchical porous carbon(HHPC)with a honeycomb-like structure by one-step carbonization method using high-yield and low-cost biomass silkworm excrement as a precursor.As an anode for SIB,HHPC-1100 exhibits a capacity of 331.7 mA h g^(-1) at 20 mA g^(-1),while it also reveals remarkable rate performance and stable long cycle capability due to its abundant pore structure and proper amount of hetero atom doping.Moreover,the synergistic effect of O,N,S,P co-doping in carbon materials on sodium ion adsorption is verified by the first-principles study,which provide a theoretical basis for the prominent electrochemical performance of the material.
基金supported by the Doctor Foundation of Bingtuan (No.2014BB004)National Natural Science Foundation of China (U130329)+1 种基金the Program for Changjiang Scholars, Innovative Research Team in University (No. IRT_15R46)the Program of Science and Technology Innovation Team in Bingtuan (No. 2015BD003)
文摘Banana peel-derived porous carbon(BPPC) was prepared from banana peel and used as an adsorbent for methyl orange(MO) wastewater removal. BPPC-MO50 is a N,S-doped BPPC obtained via secondary carbonization. The BPPC-MO50 exhibited a high specific surface area of1774.3 m^2/g. Heteroatom-doped porous carbon(PC) was successfully synthesized from the BPPC absorbed MO at high temperature and used for oxygen reduction. The BPPC-MO50 displayed the highest ORR onset potential among all carbon-based electrocatalysts, i.e., 0.93 V vs.reversible hydrogen electrode(RHE). This is the first report to describe porous carbon-activated materials from agriculture and forestry waste that is used for adsorption of dyes from wastewater via an enhanced heteroatom(N,S) content. These results may contribute to the sustainable development of dye wastewater treatment by transforming saturated PC into an effective material and has potential applications in fuel cells or as energy sources.
文摘Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Heteroatom modification is one of the most effective strategies for boosting catalytic performance,as it can regulate the physicochemical properties of host catalysts to improve their intrinsic activity.Herein,aiming to provide an overview of the impact of heteroatoms on catalytic activity at the atomic level,we present a review of the key role of heteroatoms in enhancing reaction kinetics based on the reaction pathways of the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline media.In particular,the introduction of heteroatoms can directly and indirectly optimize the interactions between the active sites and intermediates,thus improving the intrinsic activity.To clearly illustrate this influence in detail,we have summarized a series of representative heteroatom-modified electrocatalysts and discussed the important roles of heteroatoms in the OER and HER reaction pathways.Finally,some challenges and perspectives for heteroatom-modified electrodes are discussed.We hope that this review will be helpful for the development of efficient and low-cost electrocatalysts for water electrolysis and other energy conversion applications.
基金supported by the National Natural Science Foundation of China(22179065,22111530112,21875118)the Tianjin Graduate Research and Innovation Project(2022BKY018)the Ph.D.Candidate Research Innovation Fund of NKU School of Materials Science and Engineering.
文摘Hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen evolution reaction(HER)/hydrazine oxidation reaction(HzOR)kinetics,is the key step.Herein,we demonstrate the development of ultrathin P/Fe co-doped NiSe_(2) nanosheets supported on modified Ni foam(P/Fe-NiSe_(2)) synthesized through a facile electrodeposition process and subsequent heat treatment.Based on electrochemical measurements,characterizations,and density functional theory calculations,a favorable“2+2”reaction mechanism with a two-step HER process and a two-step HzOR step was fully proved and the specific effect of P doping on HzOR kinetics was investigated.P/Fe-NiSe_(2) thus yields an impressive electrocatalytic performance,delivering a high current density of 100 mA cm^(−2) with potentials of−168 and 200 mV for HER and HzOR,respectively.Additionally,P/Fe-NiSe_(2) can work efficiently for hydrazine-assisted water electrolysis and Zn-Hydrazine(Zn-Hz)battery,making it promising for practical application.
基金financially supported by the National Key Research and Development Program of China(No.2021YFA1500800)the National Natural Science Foundation of China(Nos.51825204,52072377,521888101 and 51402199)+6 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2020192)the International Partnership Program of Chinese Academy of Sciences(No.174321KYSB20200005)China Postdoctoral Science Foundation(No.2017M621137)Liaoning Revitalization Talents Program(No.XLYC2007193)the Natural Science Foundation of Liaoning Province(Nos.2021-MS-014 and 2021NLTS1210)the University Innovation Talent Foundation of Liaoning Province(No.LR2018074)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(No.KF1708)。
文摘Delafossite CuFeO_(2) is a promising photocathode material for cost-efficiently photoelectrochemical(PEC)water splitting,but the unfavorable conductivity and fast recombination dynamics of photogenerated carriers limit its PEC activity for water reduction.Here,we developed a heterostructure photocathode consisting of the Cu-doped NiO(Cu:NiO)hole selective layer(HSL)and Ni-doped CuFeO_(2)(Ni:CuFeO_(2))active layer by simply annealing a homogeneous Cu-Fe oxalate layer grown on the Ni film deposited on the fluorine doped tin oxide(FTO)substrate.The obtained heterostructure of Cu:NiO/Ni:CuFeO_(2) with enhanced charge carrier transportability and high-quality interface greatly promotes the separation of photogenerated carriers.Accordingly,the Cu:NiO/Ni:CuFeO_(2) photocathode exhibits a high photocurrent density of~0.9 mA·cm^(-2 )at 0.2 V(vs.reversible hydrogen electrode,RHE),outperforming most of the reported bare CuFeO_(2) photocathodes in the literature.And the photocurrent density can be further improved to 1.2 mA·cm^(-2) after decorating NiSx cocatalyst.
文摘A new rhodium catalyzed ring opening reaction of oxabenzonorbornadienes and its derivatives was described. This reaction forms a new carbon-nitrogen bond via an intermolecular allylic displacement of the bridgehead oxygen with a piperazine's derivatives, which proceeds with very high regioselectivity.
基金supported by the National Natural Science Foundation of China (21667016, 21267011, U1402233)~~
文摘CeO2,Ce1–xZrxO2,and Ce1–xYxO2–δ(x=0.25,0.50,0.75,and 1.00)have been rapidly synthesized to estimate their catalytic behavior in decomposing CH3SH.The role of oxygen vacancies,and the relationship between the oxygen species and catalytic properties of CeO2 and Zr‐doped and Y‐doped ceria‐based materials are investigated in detail.Combining the observed catalytic performance with the characterization results,it can be deemed that surface lattice oxygen plays a critical role in methanethiol catalytic conversion over cerium oxides.Ce0.75Zr0.25O2 shows higher catalytic activity for CH3SH decomposition due to the large amount of surface lattice oxygen,readily available oxygen species,and excellent redox properties.Ce0.75Y0.25O2–δdisplays better catalytic stability owing to the greater number of oxygen vacancies that would promote bulk lattice oxygen migration to the surface of the catalyst in order to replenish surface lattice oxygen.In addition,the results show that the difference in chemical valence between Ce and the heteroatoms would strongly influence the amount of surface lattice oxygen as well as the mobility of bulk‐phase oxygen in these catalysts,thus affecting their activity and stability.
基金financially supported by the National Natural Science Foundation of China (NSFC) (Nos. 21674007 and 21734001)the financial support from National Research Foundation (NRF) of Korea (2012M3A6A7055540 and 2015M1A2A2057506)
文摘Research on asymmetric A–D–A structured non-fullerene acceptors has lagged far behind the development of symmetric counterpart.In this contribution,by simply replacing one sulfur atom in indacenodithiophene unit with a selenium atom,an asymmetric building block Se PT and a corresponding asymmetric non-fullerene acceptor Se PT-IN have been developed.Asymmetric Se PT-IN achieved a high efficiency of 10.20% in organic solar cells when blended with PBT1-C,much higher than that of symmetric TPT-IN counterpart(8.91%).Our results demonstrated an effective heteroatom substitution strategy to develop asymmetric A–D–A structured non-fullerene acceptors.
文摘Activated carbons for electrochemical capacitor electrodes are prepared from soyabean using chemical activation with KOH. The pore size is easily controllable by changing the mass ratio between KOH and carbonized product. The as-prepared materials possess a large specific surface area, unique structure, well- developed hierarchical porosity and plentiful heteroatoms（mainly O and N）. Thus resulted in its high specific capacitance,good rate capacity and cycling stability. Moreover, attributing to worldwide availability, renewable nature and low-cost, activated carbon prepared from soyabean has a good potential in energy conversion and storage devices.
基金financially supported by the Natural Science Foundation of Hebei Province (B02020208088, H2020206514, and B2021208074)the S&T Program of Hebei Province (20544401D, 20314401D, 206Z4406G, 21314402D, 21344601D, 22344402D, and 22373709D)the Research Start-up Funding at Hebei University of Science and Technology (1181381)
文摘Carbon dioxide(CO_(2))reduction into chemicals or fuels by electrocatalysis can eff ectively reduce greenhouse gas emissions and alleviate the energy crisis.Currently,CO_(2)electrocatalytic reduction(CO_(2)RR)has been considered as an ideal way to achieve“carbon neutrality.”In CO_(2)RR,the characteristics and properties of catalysts directly determine the reaction activity and selectivity of the catalytic process.Much attention has been paid to carbon-based catalysts because of their diversity,low cost,high availability,and high throughput.However,electrically neutral carbon atoms have no catalytic activity.Incorpo-rating heteroatoms has become an eff ective strategy to control the catalytic activity of carbon-based materials.The doped carbon-based catalysts reported at present show excellent catalytic performance and application potential in CO_(2)RR.Based on the type and quantity of heteroatoms doped into carbon-based catalysts,this review summarizes the performances and catalytic mechanisms of carbon-based materials doped with a single atom(including metal and without metal)and multi atoms(including metal and without metal)in CO_(2)RR and reveals prospects for developing CO_(2)electroreduction in the future.
基金the financial support from the National Natural Science Foundation of China(22108044,22208061)the Research and Development Program in Key Fields of Guangdong Province(2020B1111380002)+1 种基金the Basic Research and Applicable Basic Research in Guangzhou City(202201010290)the financial support from the Guangdong Provincial Key Laboratory of Plant Resources Biorefinery(2021GDKLPRB07)。
文摘Amorphous carbons are promising anodes for high-rate potassium-ion batteries.Most low-temperature annealed amorphous carbons display unsatisfactory capacities.Heteroatom-induced defect engineering of amorphous carbons could enhance their reversible capacities.Nevertheless,most lignocellulose biomasses lack heteroatoms,making it a challenge to design highly heteroatom-doped carbons(>10 at%).Herein,we report a new preparation strategy for amorphous carbon anodes.Nitrogen/sulfur co-doped lignin-derived porous carbons(NSLPC)with ultra-high nitrogen doping levels(21.6 at%of N and 0.8 at%of S)from renewable lignin biomacromolecule precursors were prepared through a supramolecule-mediated pyrolysis strategy.This supermolecule/lignin composite decomposes forming a covalently bonded graphitic carbon/amorphous carbon intermediate product,which induces the formation of high heteroatom doping in the obtained NSLPC.This unique pyrolysis chemistry and high heteroatom doping of NSLPC enable abundant defective active sites for the adsorption of K+and improved kinetics.The NSLPC anode delivered a high reversible capacity of 419 mAh g^(-1)and superior cycling stability(capacity retention of 96.6%at 1 A g^(-1)for 1000 cycles).Potassiumion hybrid capacitors assembled by NSLPC anode exhibited excellent cycling stability(91%capacity retention for 2000 cycles)and a high energy density of 71 Wh kg^(-1)at a power density of 92 W kg^(-1).
基金supported by the National Natural Science Foundation of China(52272296,51502092)the Fundamental Research Funds for the Central Universities(JKD01211601,1222201718002)+1 种基金the National Overseas High-Level Talent Youth Program in Chinathe Eastern Scholar Project of Shanghai。
文摘Non-graphitized carbon(NGC)has been extensively utilized as carbonaceous anode in sodium-ion batteries(SIBs).However,more optimization to achieve competitive capacity and stability is still challenging for SIBs.In the study,the dopant strategy is utilized to construct nitrogen/sulfur-doped non-graphitized carbon(N-NGC or S-NGC)shell decorated on three-dimensional graphene foam(GF)as a self-support electrode.The highly disordered microstructures of heteroatom doped carbons are produced by applying a low-temperature pyrolysis treatment to precursors containing nitrogen and sulfur.The DFT calculations of Na-ion adsorption energies at diverse heteroatom sites show marginal-S,pyrrolic N and pyridinic N with more intensive Na-ion adsorption ability than middle-S,C=O and pristine carbon.The N-NGC with dominant small graphitic regions delivers adsorption ability to Na-ion,while the S-NGC with significant single carbon lattice stripes demonstrates redox reaction with Na-ion.Evidently,in comparison with only adsorption-driven slope regions at high potential for N-NGC,the redox reaction-generated potentialplateau enables non-graphitized S-NGC superior discharge/charge capacity and cycle-stability in the slope region.This work could provide deep insight into the rational design of non-graphitized carbon with rich microstructure and composition.
