By manipulating the distribution of surface electrons,defect engineering enables effective control over the adsorption energy between adsorbates and active sites in the CO_(2)reduction reaction(CO_(2)RR).Herein,we rep...By manipulating the distribution of surface electrons,defect engineering enables effective control over the adsorption energy between adsorbates and active sites in the CO_(2)reduction reaction(CO_(2)RR).Herein,we report a hollow indium oxide nanotube containing both oxygen vacancy and sulfur doping(V_o-Sx-In_(2)O_(3))for improved CO_(2)-to-HCOOH electroreduction and Zn-CO_(2)battery.The componential synergy significantly reduces the*OCHO formation barrier to expedite protonation process and creates a favorable electronic micro-environment for*HCOOH desorption.As a result,the CO_(2)RR performance of Vo-Sx-In_(2)O_(3)outperforms Pure-In_(2)O_(3)and V_o-In_(2)O_(3),where V_o-S53-In_(2)O_(3)exhibits a maximal HCOOH Faradaic efficiency of 92.4%at-1,2 V vs.reversible hydrogen electrode(RHE)in H-cell and above 92%over a wide window potential with high current density(119.1 mA cm^(-2)at-1.1 V vs.RHE)in flow cell.Furthermore,the rechargeable Zn-CO_(2)battery utilizing V_o-S53-In_(2)O_(3)as cathode shows a high power density of 2.29 mW cm^(-2)and a long-term stability during charge-discharge cycles.This work provides a valuable perspective to elucidate co-defective catalysts in regulating the intermediates for efficient CO_(2)RR.展开更多
Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a k...Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a key factor to achieve their high electrochemical performance.Here,the effects of nanopores and sulfur doping on carbon-based nanoporous host(CNH)electrode materials for LMAs were investigated using natural polymer-derived CNHs.Homogeneous pore-filling behaviors of lithium metal in the nanopores of the CNH electrode materials were first observed by ex situ scanning electron microscopy analysis,where the protective lithium metal nucleation and growth process led to significantly high Coulombic efficiency(CE)of~99.4%and stable 600 cycles.In addition,a comparison study of CNH and sulfurdoped CNH(S-CNH)electrodes,which differ only in the presence or absence of sulfur,revealed that sulfur doping can cause lower electrochemical series resistance,higher CE value,and better cycling stability in a wide range of current densities and number of cycles.Moreover,S-CNH-based LMAs showed high electrochemical performance in full-cell Li-S battery tests using a sulfur copolymer cathode,where a high energy density of 1370Wh kgelectrode−1 and an excellent power density of 4120Wkgelectrode−1 were obtained.展开更多
We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni ...We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni Fe-LDHs was studied and the optimal surface S content was ca. 0.43 at%. The developed S-doped Ni Fe-LDH exhibits excellent OER catalyst activity in 1.0 M KOH with overpotential of only 257 m V at the current density of 10 m A cm^-2. Moreover, the catalyst could maintain high activity after 30 h stability test. The high activity of the S-doped Ni Fe-LDH catalysts may originate from the synergistic effect between S and the Fe sites. This work provides a simple but efficient way to improve the OER performance of transition metal oxides/(oxy)hydroxides.展开更多
Carbonaceous materials are promising anode candidates for potassium-ion batteries(PIBs)given its high conductivity,stable property,and abundant resource,while its practical implementation is still hampered by its limi...Carbonaceous materials are promising anode candidates for potassium-ion batteries(PIBs)given its high conductivity,stable property,and abundant resource,while its practical implementation is still hampered by its limited capacity and inferior rate behavior.Herein,we report a superior carbonaceous anode through a combined strategy of carbon hybridization and heteroatom doping.In this composite,hollow carbon spindles(HCS)were anchored on the surface of graphene(G)followed with sulfur doping treatment,aiming to integrate the high conductivity of graphene,the good structure stability of HCS,and the S doping-induced ample active sites.As a PIB anode,the S-G@HCS composite can display high capacity(301 mAh g^(-1)at 0.1 A g^(-1)after 500 cycles)and long-term cyclability up to 1800 cycles at 2 A g^(-1).Impressively,it can deliver an outstanding rate capacity of 215 mAh g^(-1)at 10 A g^(-1),which is superior to most carbon anodes as-reported so far for PIBs.Experimental and theoretical analysis manifests that the construction of graphene/amorphous carbon interface as well as S doping enables the regulation of electronic structure and ion adsorption/transportation properties of carbonaceous material,thus accounting for the high capacity and superior rate capability of S-G@HCS composite.展开更多
Alkaline seawater electrolysis is promising for large-scale production of green hydrogen but the chlorine evolution reaction(CER)causes severe anode’s corrosion under high current densities.This work described the us...Alkaline seawater electrolysis is promising for large-scale production of green hydrogen but the chlorine evolution reaction(CER)causes severe anode’s corrosion under high current densities.This work described the use of a sulfur-doped NiFe layered double hydroxide nanoarray on Ni foam(S-NiFe LDH/NF)synthesized through a two-step hydrothermal process as a durable catalyst for alkaline seawater oxidation.In 1 M KOH+seawater,the S-NiFe LDH/NF anode needs a low overpotential of 345 mV to afford a current density of 1000 mA·cm^(-2)and operates stably over 800 h.Sulfate species generated on the catalyst surface,which is evidenced by in situ Raman spectroscopy analysis,electrostatically repel Cl^(−)and thus inhibits the CER.Furthermore,the two-electrode system using S-NiFe LDH/NF and Pt/C/NF as the anode and cathode,respectively,requires a cell voltage of 1.90 V to achieve a current density of 100 mA·cm^(-2)and maintains stable operation for 1000 h at 500 mA·cm^(-2)in alkaline seawater.展开更多
Hard carbon(HC)in sodium-ion batteries is searched by numerous investigations,which can offer the excellent performance of reversible Na^(+)insertion and extraction.The covalent heteroatom doping in HC is recently wor...Hard carbon(HC)in sodium-ion batteries is searched by numerous investigations,which can offer the excellent performance of reversible Na^(+)insertion and extraction.The covalent heteroatom doping in HC is recently worth concentrating,which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes.However,the reported doping strategies of the modified HC have only resulted in limited improvement,especially unobvious effects on tuning porous structure.In this study,tannin extract and K_(2)SO_(4) are respectively utilized as carbon source and sulfur source for the fabrication of HC,in which K_(2)SO_(4) can contribute to the heteroatom doping,and the pore forming as well.The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability,achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g.Even after 500 cycles at a current density of 3 A/g,a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6%can be reserved.Compared with the initial carbon,the adsorption energy of Na^(+)is multifold times higher,whereas Na^(+)diffusion energy barriers manyfold decrease.Moreover,the full battery assembled with Na_(3)V_(2)(PO_(4))_(3)/tannin-based HC demonstrates a stable cycling performance.This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries(SIBs),which could especially offer an explanation of Na^(+)storage and solid-electrolyte interface(SEI)stability to the electrochemical performance.展开更多
Regulation of the second nearest neighbor coordination atoms is a potent strategy for enhancing electrocatalytic oxygen reduction reaction(ORR)activity of manganese-nitrogen-carbon(Mn–N–C)catalysts with Mn–N_(4)sit...Regulation of the second nearest neighbor coordination atoms is a potent strategy for enhancing electrocatalytic oxygen reduction reaction(ORR)activity of manganese-nitrogen-carbon(Mn–N–C)catalysts with Mn–N_(4)sites.However,precisely regulating the second-nearest neighbor coordination environment of the Mn site is still challenging.Here,a novel approach is proposed to modulate the local microenvironment of Mn–N_(4)sites by strategically doping sulfur(S)atoms at the second nearest neighbor coordination positions to address this challenge.Density functional theory calculations elucidate that S-doping at these positions significantly alters the charge distribution of the Mn site,inducing a downshift in the d-band center of Mn.This electronic modulation weakens the binding strength of the Mn site toward the*OH intermediate,thereby reducing the energy barrier for the ORR process.To experimentally realize this concept,the strategic molecular assembly approach is employed to precisely incorporate S atoms into the second nearest neighbor coordination of the Mn site,resulting in the construction of the manganese-nitrogen-sulfur-carbon(Mn–N–S–C)catalysts.The Mn–N–S–C showcases a favorable halfwave potential of 0.913 V.When integrated into rechargeable liquid zinc-air batteries(ZABs)the Mn–N–S–C-based ZABs deliver high power density of 209.8 mW cm^(-2)and stable cycling performance for 800 h.Furthermore,Mn–N–S–C-based quasi-solid-state ZABs exhibit a power density of 34.05 m W cm^(-2)and a cycle life of 23 h.This study highlights the importance of the second nearest neighbor coordination atoms in tuning the electronic structure of single atom active sites,proposes a method to enhance ORR efficiency through atomic-level engineering,and demonstrates the practical application of the Mn–N–S–C catalyst in high-performance energy storage systems.These findings provide valuable insights into the design principles for next-generation catalyst design and support advancements in energy conversion and storage technologies.展开更多
A series of diamonds with boron and sulfur co-doping were synthesized in the Fe Ni Mn Co-C system by temperature gradient growth（TGG） under high pressure and high temperature（HPHT）. Because of differences in addit...A series of diamonds with boron and sulfur co-doping were synthesized in the Fe Ni Mn Co-C system by temperature gradient growth（TGG） under high pressure and high temperature（HPHT）. Because of differences in additives, the resulting diamond crystals were colorless, blue-black, or yellow. Their morphologies were slab, tower, or minaret-like. Analysis of the x-ray photoelectron spectra（XPS） of these diamonds shows the presence of B, S, and N in samples from which N was not eliminated. But only the B dopant was assuredly incorporated in the samples from which N was eliminated. Resistivity and Hall mobility were 8.510 Ω·cm and 760.870 cm^2/V·s, respectively, for a P-type diamond sample from which nitrogen was eliminated. Correspondingly, resistivity and Hall mobility were 4.211×10^5 Ω·cm and 76.300 cmΩ2/V·s for an N-type diamond sample from which nitrogen was not eliminated. Large N-type diamonds of type Ib with B–S doping were acquired.展开更多
Lithium metal batteries(LMBs)have attracted great intention due to the high energy density[1].Among various battery technologies,lithium-sulfur(Li-S)batteries are also very unique but important due to its high energy ...Lithium metal batteries(LMBs)have attracted great intention due to the high energy density[1].Among various battery technologies,lithium-sulfur(Li-S)batteries are also very unique but important due to its high energy density,low cost and available sources[2].Although Li-s batteries exhibit high energy density,the cycling life is poor,especially for large-capacity pouch cells[3].The cycling performance of Li-s batteries is crucially determined by 16-electron complex sulfur reduction reaction(SRR)from S_(8)molecules to Li_(2)S,solid,which involves the multiple potential interwoven branches among lithium polysulfide intermediates(LiPS,e.g.,S_(8),Li_(2)S_(8),Li_(2)S_(6),Li_(2)S_(4)and Li_(2)S)[4].The obvious shuttle for soluble Lips across the cathode and anode leads to the battery capacity fading.Thus,it is necessary to decrease the accumulation of soluble Lips in the electrolyte through catalysts fastening the key conversion step from high-order polysulfides to insoluble Li_(2)S_(2)/Li_(2)S.Although some effort has been devoted to catalyze SRR,the complex mechanism remains unclear.To address this issue,Duan et al.tried to solve it based on nitrogen,sulfur,dualdoped holey graphene framework(N,S-HGF)electrocatalyst in Nature[5].展开更多
Carbonaceous materials are regarded as a promising anode material for potassium ion batteries(PIBs)due to their high electronic conductivity, abundant resources and low cost. However, relatively low storage capacity a...Carbonaceous materials are regarded as a promising anode material for potassium ion batteries(PIBs)due to their high electronic conductivity, abundant resources and low cost. However, relatively low storage capacity and structural instability still hinder their practical application. Herein, high sulfur-doped hard carbon(SHC-3) with a sulfur up to 27.05 at% is synthesized from polystyrene and sulfur as precursors. As an anode for PIBs, the SHC-3 delivers a superb cycling stability and rate performance(298.1 mAh g^(-1)at 100 mA g^(-1) for 1000 cycles, a capacity retention of 95.2%;220.2 mAh g^(-1)at 500 mA g^(-1) after 5200 cycles). The potassium storage of SHC-3 exhibits excellent cyclic stability at both low and high rates.Structure and kinetic studies demonstrate that the larger interlayer spacing(0.382 nm) of the SHC-3 accelerates the diffusion of potassium ions and effectively alleviates the volume expansion, and thus maintains the structure stability during the process of potassization/de-potassization. Meanwhile, the density functional theory calculation shows that the doped sulfur atoms provide abundant active sites for the adsorption of potassium ions, thereby increasing the reversible capacity of PIBs. This work provides a new scheme for the design of carbonaceous anode materials with high capacity and long cycle life.展开更多
The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur precursors.The wet impregnation technique successfully prepared carbon material carrier...The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur precursors.The wet impregnation technique successfully prepared carbon material carriers doped with varying sources of sulfur(Na_(2)SO_(4),NaHSO_(3),Na_(2)S·9H_(2)O).Palladium carbon catalysts doped with different sulfur precursors had been prepared with the aid of the liquid-phase reduction method of the selective hydrogenation of o-chloronitrobenzene(o-CNB)to o-chloroaniline(o-CAN).The catalyst prepared for Na_(2)S·9H_(2)O as a precursor has excellent performance,and the selectivity for o-CAN is more than 99.9%at 100%conversion.In addition,the characterization results show that with the decrease of S valence,the electronic effect between S and Pd increases,and the outer electron shift of Pd increases,which reduces the adsorption and dissociation ability of Pd to hydrogen,resulting in excellent selectivity.The effects provided a good idea for the hydrogenation of o-CNB and a different point of view on sulfur doping in a variety of hydrogenation reactions.展开更多
Sulfur doped carbonaceous materials are promising anodes for potassium-ion batteries because of their ability to bridge active sites and induce C/S electron coupling,resulting in increased ion storage capacitance Howe...Sulfur doped carbonaceous materials are promising anodes for potassium-ion batteries because of their ability to bridge active sites and induce C/S electron coupling,resulting in increased ion storage capacitance However,the large potassium ions could cause significant volume expansion and structure collapse during operation in sulfur doped carbonaceous anodes,which lead to rapidly capacity sacrifice during long-term cycling.Nanopore design for anchoring sulfur atom in carbon skeleton is a novel way to alleviate the structure collapse and maintain the cycling stability.Therefore,this study developed a controlled nanopore and sulfur doped carbon sphere structure(S-NPHCSs).In potassium-ion batteries S-NPHCSs anode demonstrated exceptional performance with a high reversible capacity of 247 mAh·g^(–1)after 50 cycles at 0.2 A·g^(–1)and delivered a long cycle stability of 600 cycles at a high current density of 1.0 A·g^(–1).Interconnected nanopores and doped sulfur structure not only expand the accumulation space and offer ample active sites for diffusion and adsorption of potassium ions,but also build stable channels through nanopore structure to ensure the cyclic stability.This finding provides a fundamental theory for designing nanopore structures and introducing sulfur doped carbonaceous materials to enhance capacitive potassium storage and long cycle stability.展开更多
Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,r...Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,real-time and efficient technique.Herein,novel sulfur-doped mesoporous WO_(3)materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering,which possessed highly crystallized frameworks,high specific surface area(40.9–63.8 m^(2)/g)and uniform pore size(~18 nm).Benefitting from abundant oxygen vacancy and defects via S-doping,the tailored mesoporous S/m WO_(3)exhibited excellent benzene sensing performance,including high sensitivity(50 ppm vs.48),low detection limit(ca.500 ppb),outstanding selectivity and favorable stability.In addition,the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing interfaces.It provides brand-new approach to design sensitive materials with multiple reaction sites.展开更多
Pseudo-capacitive mechanisms can provide higher energy densities than electrical double-layer capacitors while being faster than bulk storage mechanisms.Usually,they suffer from low intrinsic electronic and ion conduc...Pseudo-capacitive mechanisms can provide higher energy densities than electrical double-layer capacitors while being faster than bulk storage mechanisms.Usually,they suffer from low intrinsic electronic and ion conductivities of the active materials.Here,taking advantage of the combination of TiS2 decoration,sulfur doping,and a nanometer-sized structure,as-spun TiO2/C nanofiber composites are developed that enable rapid transport of sodium ions and electrons,and exhibit enhanced pseudo-capacitively dominated capacities.At a scan rate of 0.5 mV s−1,a high pseudo-capacitive contribution(76%of the total storage)is obtained for the S-doped TiS2/TiO2/C electrode(termed as TiS2/S-TiO2/C).Such enhanced pseudocapacitive activity allows rapid chemical kinetics and significantly improves the high-rate sodium storage performance of TiO2.The TiS2/S-TiO2/C composite electrode delivers a high capacity of 114 mAh g−1 at a current density of 5000 mA g−1.The capacity maintains at high level(161 mAh g−1)even after 1500 cycles and is still characterized by 58 mAh g−1 at the extreme condition of 10,000 mA g−1 after 10,000 cycles.展开更多
A nanoporous N-doped reduced graphene oxide（p-N-rGO） was prepared through carbothermal reaction between graphene oxide and ammonium-containing oxometalates as sulfur host for Li-S batteries.The p-N-rGO sheets have a...A nanoporous N-doped reduced graphene oxide（p-N-rGO） was prepared through carbothermal reaction between graphene oxide and ammonium-containing oxometalates as sulfur host for Li-S batteries.The p-N-rGO sheets have abundant nanopores with diameters of 10-40 nm and the nitrogen content is 2.65 at%.When used as sulfur cathode,the obtained p-N-rGO/S composite has a high reversible capacity of 1110mAhg^-1 at 1C rate and stable cycling performance with 781.8 mAhg-1 retained after 110 cycles,much better than those of the rGO/S composite.The enhanced electrochemical performance is ascribed to the rational combination of nanopores and N-doping,which provide efficient contact and wetting with the electrolyte,accommodate volume expansion and immobilize polysulfides during cycling.展开更多
Coupling the thermodynamically favorable sulfion oxidation reaction(SOR)with the hydrogen evolution reaction(HER)is a promising approach to simultaneously save energy and cost-effectively produce high value-added chem...Coupling the thermodynamically favorable sulfion oxidation reaction(SOR)with the hydrogen evolution reaction(HER)is a promising approach to simultaneously save energy and cost-effectively produce high value-added chemicals and hydrogen.The construction of efficient bifunctional catalysts for SOR-HER electrocatalysis is of significance yet challenging.展开更多
At present, the problem of electromagnetic wave(EMW) pollution is critical, and the design of highperformance absorbers is of great significance. Based on the synergy between dielectric and magnetic losses, and betwee...At present, the problem of electromagnetic wave(EMW) pollution is critical, and the design of highperformance absorbers is of great significance. Based on the synergy between dielectric and magnetic losses, and between multicomponents in heterostructures, the development of light-weight absorbers with a strong absorption capability and multiple scattering is a promising strategy to achieve highperformance absorbers. In this work, CoFe-MOF precursors with a bouquet-like structure were prepared via the hydrothermal method, and Co_(7)Fe_(3)/C and Co_(9)S_(8)/FeCoS_(2)/C composites were obtained through a carbonization and sulfuration treatment during the high-temperature pyrolysis process, respectively. The experimental and theoretical results show that the Co_(9)S_(8)/FeCoS_(2)/C composite has a better EMW absorption performance, and its optimal reflection loss(RL) value is-53.9 d B at a low filler loading of 20 wt.%,which is due to the S doping that enhances the interface polarization relaxation process and improves the impedance matching characteristics. Moreover, the Co_(9)S_(8)/FeCoS_(2)/C composite can be as candidates of high-efficiency absorbers in extreme application environments.展开更多
Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-s...Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-substrate interaction.Herein,atomically dispersed Fe-NC material with precise sulfur modification to Fe periphery(termed as Fe-NSC) was synthesized,X-ray absorption near edge structure analysis confirmed the central Fe atom being stabilized in a specific configuration of Fe(N3)(N-C-S).By enabling precisely localized S doping,the electronic structure of Fe-N4 moiety could be mediated,leading to the beneficial adjustment of absorption/desorption properties of reactant/intermediate on Fe center.Density functional theory simulation suggested that more negative charge density would be localized over Fe-N4 moiety after S doping,allowing weakened binding capability to *OH intermediates and faster charge transfer from Fe center to O species.Electrochemical measurements revealed that the Fe-NSC sample exhibited significantly enhanced oxygen reduction reaction performance compared to the S-free Fe-NC material(termed as Fe-NC),showing an excellent onset potential of 1.09 V and half-wave potential of 0.92 V in 0.1 M KOH.Our work may enlighten relevant studies regarding to accessing improvement on the catalytic performance of atomically dispersed M-NC materials by managing precisely tuned local environments of M-Nx moiety.展开更多
Heteroatom-doped carbon-based transition-metal single-atom catalysts(SACs) are promising electrocatalysts for oxygen reduction reaction(ORR). Herein, with the aid of hierarchically porous silica as hard template, a fa...Heteroatom-doped carbon-based transition-metal single-atom catalysts(SACs) are promising electrocatalysts for oxygen reduction reaction(ORR). Herein, with the aid of hierarchically porous silica as hard template, a facile and general melting perfusion and mesopore-confined pyrolysis method was reported to prepare single-atomic Fe/N–S-doped carbon catalyst(FeNx/NC-S) with hierarchically porous structure and well-defined morphology. The FeNx/NC-S exhibited excellent ORR activity with a half-wave potential(E_(1/2)) of 0.92 V, and a lower overpotential of 320 mV at a current density of 10 mA cm^(-2)for OER under alkaline condition. The remarkable electrocatalysis performance can be attributed to the hierarchically porous carbon nanospheres with S doping and high content of Fe-Nx sites(up to 3.7 wt% of Fe), resulting from the nano-confinement effect of the hierarchically porous silica spheres(NKM-5) during the pyrolysis process. The rechargeable Zn-air battery with FeNx/NC-S as a cathode catalyst demonstrated a superior power density of 194.5 mW cm-2charge–discharge stability. This work highlights a new avenue to design advanced SACs for efficient sustainable energy storage and conversion.展开更多
Anatase TiO_2 has been investigated as one of the most promising anode materials for sodium ion batteries(SIBs)with low cost and high theoretical capacity.Herein,a composite material of TiO_2 /N,S-RGO@C with carbon co...Anatase TiO_2 has been investigated as one of the most promising anode materials for sodium ion batteries(SIBs)with low cost and high theoretical capacity.Herein,a composite material of TiO_2 /N,S-RGO@C with carbon coated ultrasmall anatase TiO_2 anchored on nitrogen and sulfur co-doped RGO matrix was successfully prepared by a rational designed process.The composite structure exhibited ultrasmall crystal size,rich porous structure,homogeneous heteroatoms doping and thin carbon coating,which synergistically resulted in elevated electron and ion transfer.The anode exhibited high rate capacities with good reversibility under high rate cycling.The carbon coating was investigated to be effective to prevent active material falling and lead to long term cycling performance with a high capacity retention of 181 m Ah g^(à1)after 2000cycles at 2 C.Kinetic studies were carried out and the results revealed that the superior performance of the composite material were derived from the decreased charge transfer resistance and elevated ion diffusion.Results suggested that the TiO_2 /N,S-RGO@C composite is a promising anode material for sodium ion batteries.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(22120230104).
文摘By manipulating the distribution of surface electrons,defect engineering enables effective control over the adsorption energy between adsorbates and active sites in the CO_(2)reduction reaction(CO_(2)RR).Herein,we report a hollow indium oxide nanotube containing both oxygen vacancy and sulfur doping(V_o-Sx-In_(2)O_(3))for improved CO_(2)-to-HCOOH electroreduction and Zn-CO_(2)battery.The componential synergy significantly reduces the*OCHO formation barrier to expedite protonation process and creates a favorable electronic micro-environment for*HCOOH desorption.As a result,the CO_(2)RR performance of Vo-Sx-In_(2)O_(3)outperforms Pure-In_(2)O_(3)and V_o-In_(2)O_(3),where V_o-S53-In_(2)O_(3)exhibits a maximal HCOOH Faradaic efficiency of 92.4%at-1,2 V vs.reversible hydrogen electrode(RHE)in H-cell and above 92%over a wide window potential with high current density(119.1 mA cm^(-2)at-1.1 V vs.RHE)in flow cell.Furthermore,the rechargeable Zn-CO_(2)battery utilizing V_o-S53-In_(2)O_(3)as cathode shows a high power density of 2.29 mW cm^(-2)and a long-term stability during charge-discharge cycles.This work provides a valuable perspective to elucidate co-defective catalysts in regulating the intermediates for efficient CO_(2)RR.
基金National Research Foundation of Korea,Grant/Award Numbers:2019R1A2C1084836,2021R1A4A2001403。
文摘Studies on three-dimensional structured carbon templates have focused on how to guide homogeneous lithium metal nucleation and growth for lithium metal anodes(LMAs).However,there is still insufficient evidence for a key factor to achieve their high electrochemical performance.Here,the effects of nanopores and sulfur doping on carbon-based nanoporous host(CNH)electrode materials for LMAs were investigated using natural polymer-derived CNHs.Homogeneous pore-filling behaviors of lithium metal in the nanopores of the CNH electrode materials were first observed by ex situ scanning electron microscopy analysis,where the protective lithium metal nucleation and growth process led to significantly high Coulombic efficiency(CE)of~99.4%and stable 600 cycles.In addition,a comparison study of CNH and sulfurdoped CNH(S-CNH)electrodes,which differ only in the presence or absence of sulfur,revealed that sulfur doping can cause lower electrochemical series resistance,higher CE value,and better cycling stability in a wide range of current densities and number of cycles.Moreover,S-CNH-based LMAs showed high electrochemical performance in full-cell Li-S battery tests using a sulfur copolymer cathode,where a high energy density of 1370Wh kgelectrode−1 and an excellent power density of 4120Wkgelectrode−1 were obtained.
文摘We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni Fe-LDHs was studied and the optimal surface S content was ca. 0.43 at%. The developed S-doped Ni Fe-LDH exhibits excellent OER catalyst activity in 1.0 M KOH with overpotential of only 257 m V at the current density of 10 m A cm^-2. Moreover, the catalyst could maintain high activity after 30 h stability test. The high activity of the S-doped Ni Fe-LDH catalysts may originate from the synergistic effect between S and the Fe sites. This work provides a simple but efficient way to improve the OER performance of transition metal oxides/(oxy)hydroxides.
基金supported by National Natural Science Foundation of China(Grant 61935017,21701174,21771182)Projects of International Cooperation and Exchanges NSFC(Grant 51811530018)+2 种基金Synergetic Innovation Center for Organic Electronics and Information Displaysthe Youth Innovation Promotion Associa tion CASthe start-up funding from FJNU。
文摘Carbonaceous materials are promising anode candidates for potassium-ion batteries(PIBs)given its high conductivity,stable property,and abundant resource,while its practical implementation is still hampered by its limited capacity and inferior rate behavior.Herein,we report a superior carbonaceous anode through a combined strategy of carbon hybridization and heteroatom doping.In this composite,hollow carbon spindles(HCS)were anchored on the surface of graphene(G)followed with sulfur doping treatment,aiming to integrate the high conductivity of graphene,the good structure stability of HCS,and the S doping-induced ample active sites.As a PIB anode,the S-G@HCS composite can display high capacity(301 mAh g^(-1)at 0.1 A g^(-1)after 500 cycles)and long-term cyclability up to 1800 cycles at 2 A g^(-1).Impressively,it can deliver an outstanding rate capacity of 215 mAh g^(-1)at 10 A g^(-1),which is superior to most carbon anodes as-reported so far for PIBs.Experimental and theoretical analysis manifests that the construction of graphene/amorphous carbon interface as well as S doping enables the regulation of electronic structure and ion adsorption/transportation properties of carbonaceous material,thus accounting for the high capacity and superior rate capability of S-G@HCS composite.
文摘Alkaline seawater electrolysis is promising for large-scale production of green hydrogen but the chlorine evolution reaction(CER)causes severe anode’s corrosion under high current densities.This work described the use of a sulfur-doped NiFe layered double hydroxide nanoarray on Ni foam(S-NiFe LDH/NF)synthesized through a two-step hydrothermal process as a durable catalyst for alkaline seawater oxidation.In 1 M KOH+seawater,the S-NiFe LDH/NF anode needs a low overpotential of 345 mV to afford a current density of 1000 mA·cm^(-2)and operates stably over 800 h.Sulfate species generated on the catalyst surface,which is evidenced by in situ Raman spectroscopy analysis,electrostatically repel Cl^(−)and thus inhibits the CER.Furthermore,the two-electrode system using S-NiFe LDH/NF and Pt/C/NF as the anode and cathode,respectively,requires a cell voltage of 1.90 V to achieve a current density of 100 mA·cm^(-2)and maintains stable operation for 1000 h at 500 mA·cm^(-2)in alkaline seawater.
基金supported by National Natural Science Foundation of China(Nos.32271791,32171709 and 22475053)Hunan Provincial Natural Science Foundation of China(No.2024JJ7643)Natural Science Foundation of Shanghai(No.22ZR1404100).
文摘Hard carbon(HC)in sodium-ion batteries is searched by numerous investigations,which can offer the excellent performance of reversible Na^(+)insertion and extraction.The covalent heteroatom doping in HC is recently worth concentrating,which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes.However,the reported doping strategies of the modified HC have only resulted in limited improvement,especially unobvious effects on tuning porous structure.In this study,tannin extract and K_(2)SO_(4) are respectively utilized as carbon source and sulfur source for the fabrication of HC,in which K_(2)SO_(4) can contribute to the heteroatom doping,and the pore forming as well.The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability,achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g.Even after 500 cycles at a current density of 3 A/g,a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6%can be reserved.Compared with the initial carbon,the adsorption energy of Na^(+)is multifold times higher,whereas Na^(+)diffusion energy barriers manyfold decrease.Moreover,the full battery assembled with Na_(3)V_(2)(PO_(4))_(3)/tannin-based HC demonstrates a stable cycling performance.This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries(SIBs),which could especially offer an explanation of Na^(+)storage and solid-electrolyte interface(SEI)stability to the electrochemical performance.
基金financially supported by the National Natural Science Foundation of China(22278193,22178148 and 22208126)the Priority Academic Program Development of Jiangsu Higher Education Institutions+1 种基金Jiangsu Funding Program for Excellent Postdoctoral Talent(2024ZB129)the Postdoctoral Fellowship Program of CPSF(GZC20240612)。
文摘Regulation of the second nearest neighbor coordination atoms is a potent strategy for enhancing electrocatalytic oxygen reduction reaction(ORR)activity of manganese-nitrogen-carbon(Mn–N–C)catalysts with Mn–N_(4)sites.However,precisely regulating the second-nearest neighbor coordination environment of the Mn site is still challenging.Here,a novel approach is proposed to modulate the local microenvironment of Mn–N_(4)sites by strategically doping sulfur(S)atoms at the second nearest neighbor coordination positions to address this challenge.Density functional theory calculations elucidate that S-doping at these positions significantly alters the charge distribution of the Mn site,inducing a downshift in the d-band center of Mn.This electronic modulation weakens the binding strength of the Mn site toward the*OH intermediate,thereby reducing the energy barrier for the ORR process.To experimentally realize this concept,the strategic molecular assembly approach is employed to precisely incorporate S atoms into the second nearest neighbor coordination of the Mn site,resulting in the construction of the manganese-nitrogen-sulfur-carbon(Mn–N–S–C)catalysts.The Mn–N–S–C showcases a favorable halfwave potential of 0.913 V.When integrated into rechargeable liquid zinc-air batteries(ZABs)the Mn–N–S–C-based ZABs deliver high power density of 209.8 mW cm^(-2)and stable cycling performance for 800 h.Furthermore,Mn–N–S–C-based quasi-solid-state ZABs exhibit a power density of 34.05 m W cm^(-2)and a cycle life of 23 h.This study highlights the importance of the second nearest neighbor coordination atoms in tuning the electronic structure of single atom active sites,proposes a method to enhance ORR efficiency through atomic-level engineering,and demonstrates the practical application of the Mn–N–S–C catalyst in high-performance energy storage systems.These findings provide valuable insights into the design principles for next-generation catalyst design and support advancements in energy conversion and storage technologies.
基金Project supported by the National Natural Science Foundation of China(Grant No.11604246)China Postdoctor Science Foundation(Grant No.2016M592714)+2 种基金Professional Practice Demonstration Base for Professional Degree Graduate in Material Engineering of Henan Polytechnic University,China(Grant No.2016YJD03)the Education Department of Henan Province,China(Grant Nos.12A430010 and 17A430020)the Fundamental Research Funds for the Universities of Henan Province,China(Grant No.NSFRF140110)
文摘A series of diamonds with boron and sulfur co-doping were synthesized in the Fe Ni Mn Co-C system by temperature gradient growth（TGG） under high pressure and high temperature（HPHT）. Because of differences in additives, the resulting diamond crystals were colorless, blue-black, or yellow. Their morphologies were slab, tower, or minaret-like. Analysis of the x-ray photoelectron spectra（XPS） of these diamonds shows the presence of B, S, and N in samples from which N was not eliminated. But only the B dopant was assuredly incorporated in the samples from which N was eliminated. Resistivity and Hall mobility were 8.510 Ω·cm and 760.870 cm^2/V·s, respectively, for a P-type diamond sample from which nitrogen was eliminated. Correspondingly, resistivity and Hall mobility were 4.211×10^5 Ω·cm and 76.300 cmΩ2/V·s for an N-type diamond sample from which nitrogen was not eliminated. Large N-type diamonds of type Ib with B–S doping were acquired.
文摘Lithium metal batteries(LMBs)have attracted great intention due to the high energy density[1].Among various battery technologies,lithium-sulfur(Li-S)batteries are also very unique but important due to its high energy density,low cost and available sources[2].Although Li-s batteries exhibit high energy density,the cycling life is poor,especially for large-capacity pouch cells[3].The cycling performance of Li-s batteries is crucially determined by 16-electron complex sulfur reduction reaction(SRR)from S_(8)molecules to Li_(2)S,solid,which involves the multiple potential interwoven branches among lithium polysulfide intermediates(LiPS,e.g.,S_(8),Li_(2)S_(8),Li_(2)S_(6),Li_(2)S_(4)and Li_(2)S)[4].The obvious shuttle for soluble Lips across the cathode and anode leads to the battery capacity fading.Thus,it is necessary to decrease the accumulation of soluble Lips in the electrolyte through catalysts fastening the key conversion step from high-order polysulfides to insoluble Li_(2)S_(2)/Li_(2)S.Although some effort has been devoted to catalyze SRR,the complex mechanism remains unclear.To address this issue,Duan et al.tried to solve it based on nitrogen,sulfur,dualdoped holey graphene framework(N,S-HGF)electrocatalyst in Nature[5].
基金financially supported by the National Natural Science Foundation of China (Grants 21975069 and 21872045)the Key Project of Research and Development Plan of Hunan Province (Grant 2019SK2071)。
文摘Carbonaceous materials are regarded as a promising anode material for potassium ion batteries(PIBs)due to their high electronic conductivity, abundant resources and low cost. However, relatively low storage capacity and structural instability still hinder their practical application. Herein, high sulfur-doped hard carbon(SHC-3) with a sulfur up to 27.05 at% is synthesized from polystyrene and sulfur as precursors. As an anode for PIBs, the SHC-3 delivers a superb cycling stability and rate performance(298.1 mAh g^(-1)at 100 mA g^(-1) for 1000 cycles, a capacity retention of 95.2%;220.2 mAh g^(-1)at 500 mA g^(-1) after 5200 cycles). The potassium storage of SHC-3 exhibits excellent cyclic stability at both low and high rates.Structure and kinetic studies demonstrate that the larger interlayer spacing(0.382 nm) of the SHC-3 accelerates the diffusion of potassium ions and effectively alleviates the volume expansion, and thus maintains the structure stability during the process of potassization/de-potassization. Meanwhile, the density functional theory calculation shows that the doped sulfur atoms provide abundant active sites for the adsorption of potassium ions, thereby increasing the reversible capacity of PIBs. This work provides a new scheme for the design of carbonaceous anode materials with high capacity and long cycle life.
基金financially supported by the National Natural Science Foundation of China(22078292,22008212,U20A20119,21776258)。
文摘The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur precursors.The wet impregnation technique successfully prepared carbon material carriers doped with varying sources of sulfur(Na_(2)SO_(4),NaHSO_(3),Na_(2)S·9H_(2)O).Palladium carbon catalysts doped with different sulfur precursors had been prepared with the aid of the liquid-phase reduction method of the selective hydrogenation of o-chloronitrobenzene(o-CNB)to o-chloroaniline(o-CAN).The catalyst prepared for Na_(2)S·9H_(2)O as a precursor has excellent performance,and the selectivity for o-CAN is more than 99.9%at 100%conversion.In addition,the characterization results show that with the decrease of S valence,the electronic effect between S and Pd increases,and the outer electron shift of Pd increases,which reduces the adsorption and dissociation ability of Pd to hydrogen,resulting in excellent selectivity.The effects provided a good idea for the hydrogenation of o-CNB and a different point of view on sulfur doping in a variety of hydrogenation reactions.
基金supported by the Key R&D Plan of Jihua Laboratory(Nos.X200191TL200 and X220301XS220)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110052)+1 种基金Foshan Postdoctoral Science Foundation(Nos.X221071MS210)Numerical computations were performed on Hefei advanced computing center。
文摘Sulfur doped carbonaceous materials are promising anodes for potassium-ion batteries because of their ability to bridge active sites and induce C/S electron coupling,resulting in increased ion storage capacitance However,the large potassium ions could cause significant volume expansion and structure collapse during operation in sulfur doped carbonaceous anodes,which lead to rapidly capacity sacrifice during long-term cycling.Nanopore design for anchoring sulfur atom in carbon skeleton is a novel way to alleviate the structure collapse and maintain the cycling stability.Therefore,this study developed a controlled nanopore and sulfur doped carbon sphere structure(S-NPHCSs).In potassium-ion batteries S-NPHCSs anode demonstrated exceptional performance with a high reversible capacity of 247 mAh·g^(–1)after 50 cycles at 0.2 A·g^(–1)and delivered a long cycle stability of 600 cycles at a high current density of 1.0 A·g^(–1).Interconnected nanopores and doped sulfur structure not only expand the accumulation space and offer ample active sites for diffusion and adsorption of potassium ions,but also build stable channels through nanopore structure to ensure the cyclic stability.This finding provides a fundamental theory for designing nanopore structures and introducing sulfur doped carbonaceous materials to enhance capacitive potassium storage and long cycle stability.
基金supported by the National Natural Science Foundation of China(Nos.22125501,U22A20152,22105043,52225204,52173233)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.20JC1415300)+1 种基金the state key laboratory of Transducer Technology of China(No.SKT2207)the Fundamental Research Funds for the Central Universities(No.20720220010)。
文摘Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,real-time and efficient technique.Herein,novel sulfur-doped mesoporous WO_(3)materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering,which possessed highly crystallized frameworks,high specific surface area(40.9–63.8 m^(2)/g)and uniform pore size(~18 nm).Benefitting from abundant oxygen vacancy and defects via S-doping,the tailored mesoporous S/m WO_(3)exhibited excellent benzene sensing performance,including high sensitivity(50 ppm vs.48),low detection limit(ca.500 ppb),outstanding selectivity and favorable stability.In addition,the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing interfaces.It provides brand-new approach to design sensitive materials with multiple reaction sites.
基金This work was financially supported by National Key R&D Program of China(No.2018YFB0905400)the National Natural Science Foundation of China(Nos.51925207,51872277,and U1910210)+2 种基金Dalian National Laboratory For Clean Energy(DNL)Cooperation Fund,the CAS(DNL180310)the Fundamental Research Funds for the Central Universities(Wk2060140026)Sofja Kovalevskaja award of the Humboldt Society.This project has received funding from the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No.823717-ESTEEM3.
文摘Pseudo-capacitive mechanisms can provide higher energy densities than electrical double-layer capacitors while being faster than bulk storage mechanisms.Usually,they suffer from low intrinsic electronic and ion conductivities of the active materials.Here,taking advantage of the combination of TiS2 decoration,sulfur doping,and a nanometer-sized structure,as-spun TiO2/C nanofiber composites are developed that enable rapid transport of sodium ions and electrons,and exhibit enhanced pseudo-capacitively dominated capacities.At a scan rate of 0.5 mV s−1,a high pseudo-capacitive contribution(76%of the total storage)is obtained for the S-doped TiS2/TiO2/C electrode(termed as TiS2/S-TiO2/C).Such enhanced pseudocapacitive activity allows rapid chemical kinetics and significantly improves the high-rate sodium storage performance of TiO2.The TiS2/S-TiO2/C composite electrode delivers a high capacity of 114 mAh g−1 at a current density of 5000 mA g−1.The capacity maintains at high level(161 mAh g−1)even after 1500 cycles and is still characterized by 58 mAh g−1 at the extreme condition of 10,000 mA g−1 after 10,000 cycles.
基金Financial support from the Research Project of National University of Defense Technology (No. ZDYYjc Yj20140701)
文摘A nanoporous N-doped reduced graphene oxide（p-N-rGO） was prepared through carbothermal reaction between graphene oxide and ammonium-containing oxometalates as sulfur host for Li-S batteries.The p-N-rGO sheets have abundant nanopores with diameters of 10-40 nm and the nitrogen content is 2.65 at%.When used as sulfur cathode,the obtained p-N-rGO/S composite has a high reversible capacity of 1110mAhg^-1 at 1C rate and stable cycling performance with 781.8 mAhg-1 retained after 110 cycles,much better than those of the rGO/S composite.The enhanced electrochemical performance is ascribed to the rational combination of nanopores and N-doping,which provide efficient contact and wetting with the electrolyte,accommodate volume expansion and immobilize polysulfides during cycling.
基金supported by the National Natural Science Foundation of China(No.21972126,21978264,21905250,and 22278369)the Natural Science Foundation of Zhejiang Province(No.LQ22B030012 and LQ23B030010)the China Postdoctoral Science Foundation(2021M702889)。
文摘Coupling the thermodynamically favorable sulfion oxidation reaction(SOR)with the hydrogen evolution reaction(HER)is a promising approach to simultaneously save energy and cost-effectively produce high value-added chemicals and hydrogen.The construction of efficient bifunctional catalysts for SOR-HER electrocatalysis is of significance yet challenging.
基金financially supported from the National Natural Science Foundation of China (Nos. 61701386 and 21975196)the Young Star Project of Science and Technology of Shaanxi Province(No. 2019KJXX-033)the Youth Innovation Team of Shaanxi Universities:Metal corrosion protection and surface engineering technology。
文摘At present, the problem of electromagnetic wave(EMW) pollution is critical, and the design of highperformance absorbers is of great significance. Based on the synergy between dielectric and magnetic losses, and between multicomponents in heterostructures, the development of light-weight absorbers with a strong absorption capability and multiple scattering is a promising strategy to achieve highperformance absorbers. In this work, CoFe-MOF precursors with a bouquet-like structure were prepared via the hydrothermal method, and Co_(7)Fe_(3)/C and Co_(9)S_(8)/FeCoS_(2)/C composites were obtained through a carbonization and sulfuration treatment during the high-temperature pyrolysis process, respectively. The experimental and theoretical results show that the Co_(9)S_(8)/FeCoS_(2)/C composite has a better EMW absorption performance, and its optimal reflection loss(RL) value is-53.9 d B at a low filler loading of 20 wt.%,which is due to the S doping that enhances the interface polarization relaxation process and improves the impedance matching characteristics. Moreover, the Co_(9)S_(8)/FeCoS_(2)/C composite can be as candidates of high-efficiency absorbers in extreme application environments.
基金supported by National Natural Science Foundation of China,Beijing University of Chemical Technology(buctrc201901)National Natural Science Foundation of China and Ministry of Foreign A airs and International Cooperation,Italy(NSFC–MAECI 51861135202)+4 种基金the National Key Research and Development Project(Grant No.2018YFB1502401,2018YFA0702002)the Royal Society and the Newton Fund through the Newton Advanced Fellowship award(NAF\R1\191294)the Program for Changjiang Scholars and Innovation Research Team in the University(No.IRT1205)the Fundamental Research Funds for the Central Universitiesthe long–term subsidy mechanism from the Ministry of Finance and the Ministry of Education of PRC。
文摘Immobilizing metal atoms by multiple nitrogen atoms has triggered exceptional catalytic activity toward many critical electrochemical reactions due to their merits of highly unsaturated coordination and strong metal-substrate interaction.Herein,atomically dispersed Fe-NC material with precise sulfur modification to Fe periphery(termed as Fe-NSC) was synthesized,X-ray absorption near edge structure analysis confirmed the central Fe atom being stabilized in a specific configuration of Fe(N3)(N-C-S).By enabling precisely localized S doping,the electronic structure of Fe-N4 moiety could be mediated,leading to the beneficial adjustment of absorption/desorption properties of reactant/intermediate on Fe center.Density functional theory simulation suggested that more negative charge density would be localized over Fe-N4 moiety after S doping,allowing weakened binding capability to *OH intermediates and faster charge transfer from Fe center to O species.Electrochemical measurements revealed that the Fe-NSC sample exhibited significantly enhanced oxygen reduction reaction performance compared to the S-free Fe-NC material(termed as Fe-NC),showing an excellent onset potential of 1.09 V and half-wave potential of 0.92 V in 0.1 M KOH.Our work may enlighten relevant studies regarding to accessing improvement on the catalytic performance of atomically dispersed M-NC materials by managing precisely tuned local environments of M-Nx moiety.
基金supported by National Natural Science Foundation of China (21773128)。
文摘Heteroatom-doped carbon-based transition-metal single-atom catalysts(SACs) are promising electrocatalysts for oxygen reduction reaction(ORR). Herein, with the aid of hierarchically porous silica as hard template, a facile and general melting perfusion and mesopore-confined pyrolysis method was reported to prepare single-atomic Fe/N–S-doped carbon catalyst(FeNx/NC-S) with hierarchically porous structure and well-defined morphology. The FeNx/NC-S exhibited excellent ORR activity with a half-wave potential(E_(1/2)) of 0.92 V, and a lower overpotential of 320 mV at a current density of 10 mA cm^(-2)for OER under alkaline condition. The remarkable electrocatalysis performance can be attributed to the hierarchically porous carbon nanospheres with S doping and high content of Fe-Nx sites(up to 3.7 wt% of Fe), resulting from the nano-confinement effect of the hierarchically porous silica spheres(NKM-5) during the pyrolysis process. The rechargeable Zn-air battery with FeNx/NC-S as a cathode catalyst demonstrated a superior power density of 194.5 mW cm-2charge–discharge stability. This work highlights a new avenue to design advanced SACs for efficient sustainable energy storage and conversion.
基金supported by the National Natural Science Foundation of China (No. 21771164 & 21671205)Henan Province (No. 15HASTIT003)Zhengzhou University (No. 1421316035)
文摘Anatase TiO_2 has been investigated as one of the most promising anode materials for sodium ion batteries(SIBs)with low cost and high theoretical capacity.Herein,a composite material of TiO_2 /N,S-RGO@C with carbon coated ultrasmall anatase TiO_2 anchored on nitrogen and sulfur co-doped RGO matrix was successfully prepared by a rational designed process.The composite structure exhibited ultrasmall crystal size,rich porous structure,homogeneous heteroatoms doping and thin carbon coating,which synergistically resulted in elevated electron and ion transfer.The anode exhibited high rate capacities with good reversibility under high rate cycling.The carbon coating was investigated to be effective to prevent active material falling and lead to long term cycling performance with a high capacity retention of 181 m Ah g^(à1)after 2000cycles at 2 C.Kinetic studies were carried out and the results revealed that the superior performance of the composite material were derived from the decreased charge transfer resistance and elevated ion diffusion.Results suggested that the TiO_2 /N,S-RGO@C composite is a promising anode material for sodium ion batteries.
