S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
ZnO thin films co-doped with A1 and Sb with different concentrations and a fixed molar ratio of AlCl3 to SbCl3 at 1:2, are prepared by a sol-gel spin-coating method on glass annealed at 550 ℃ for 2 h in air. The x-r...ZnO thin films co-doped with A1 and Sb with different concentrations and a fixed molar ratio of AlCl3 to SbCl3 at 1:2, are prepared by a sol-gel spin-coating method on glass annealed at 550 ℃ for 2 h in air. The x-ray diffraction results confirm that the ZnO thin films co-doped with Al distortion, and the biaxial stresses are 1.03× 10^8. 3.26× 10^8 and Sb are of wurtzite hexagonal ZnO with a very small 5.23 × 10^8, and 6.97× 10^8 Pa, corresponding to those of the ZnO thin films co-doped with Al and Sb in concentrations of 1.5, 3.0, 4.5, 6.0 at% respectively. The optical properties reveal that the ZnO thin films co-doped with Al and Sb have obviously enhanced transmittance in the visible region. The electrical properties show that ZnO thin film co-doped with Al and Sb in a concentration of 1.5 at% has a lowest resistivity of 2.5 Ω·cm.展开更多
Undoped and Ni–S co-doped mesoporous TiO2 nano materials were synthesized by using sol–gel method.The characteristic features of as prepared catalyst samples were investigated using various advanced spectroscopic an...Undoped and Ni–S co-doped mesoporous TiO2 nano materials were synthesized by using sol–gel method.The characteristic features of as prepared catalyst samples were investigated using various advanced spectroscopic and analytical techniques.The characterization results of the samples revealed that all the samples exhibited anatase phase(XRD),decreasing band gap(2.68 eV)(UV–Vis-DRS),small particle size(9.2 nm)(TEM),high surface area(142.156 m^2·g^-1)(BET),particles with spherical shape and smooth morphology(SEM);there is a frequency shift observed for co-doped sample(FT-IR)and the elemental composition electronic states and position of the doped elements(Ni and S)in the TiO2 lattice analyzed by XPS and EDX.These results supported the photocatalytic degradation of Bismarck Brown Red(BBR)achieved with in 110 min and also exhibited the antibacterial activity on Staphylococcus aureus(MTCC-3160),Pseudomonas fluorescence(MTCC-1688)under visible light irradiation.展开更多
Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples w...Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.展开更多
This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)w...This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)with different content(mCu-xNP/AC)were manufactured and applied in the acetylene hydrochlorination reaction.It was found that the doping of carriers N and P induced the transformation of Cu^(2+)to Cu^(+),and the catalytic activity was markedly improved.Under the optimal reaction temperature of 220℃,the gas hourly space velocity(GHSV)of C_(2)H_(2)was 90 h^(-1)and V_(HCl):V_(C_(2)H_(2))was 1.15.The initial activity of the 5%Cu-30 NP/AC catalyst reached 95.59%.Through some characterization methods showed the addition of N and P improved the dispersion of Cu in carbon,which increased the ratio of Cu^+/Cu^(2+).The measurement results confirmed that the chemisorption capacity of mCu-xNP/AC for C_(2)H_(2)decreased slightly,and the chemisorption capacity for HCl increased significantly,which was the reason for the increased activity of the catalyst.The conclusion provides a reference for the development of acetylene hydrochlorination Cu catalyst.展开更多
In the present work it is studied the phosphorus-aluminum co-doping effect on the electronic and structural graphene properties using ab initio calculations in the framework of DFT (density functional theory). The d...In the present work it is studied the phosphorus-aluminum co-doping effect on the electronic and structural graphene properties using ab initio calculations in the framework of DFT (density functional theory). The doping of graphene with substituent heteroatoms can modify the band structures as well as the electron transfer, improving the electronic performance that could enhance the sensing ability in gas sensor devices. The incorporation of heteroatoms in the graphene monolayer alters the unit cell. The alteration degree depends on the dopant concentration. Furthermore, the electronic properties were modified by opening the gap up to 0.61 eV produced by the combination of phosphorus and aluminum as dopants. The dopant concentration can be controlled, which causes different degrees of semiconductor behavior on the co-doped graphene.展开更多
Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only sh...Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium.展开更多
Heteroatom doping has emerged as a prevailing strategy to enhance the storage of sodium ions in carbon materials.However,the underlying mechanism governing the performance enhancement remains undisclosed.Herein,we fab...Heteroatom doping has emerged as a prevailing strategy to enhance the storage of sodium ions in carbon materials.However,the underlying mechanism governing the performance enhancement remains undisclosed.Herein,we fabricated N/S co-doped carbon beaded fibers(S-N-CBFs),which exhibited glorious rate performance and durableness in Na+storage,showcasing no obvious capacity decay even after 3500 cycles.Furthermore,when used as anodes in sodium-ion capacitors,the S-N-CBFs delivered exceptional results,boasting a high energy density of 225 Wh·kg^(-1),superior power output of 22500 W·kg^(-1),and outstanding cycling stability with a capacity attenuation of merely 0.014%per cycle after 4000 cycles at 2 A·g^(-1).Mechanistic investigations revealed that the incorporation of both pyridinic N and pyrrolic N into the carbon matrix of S-N-CBFs induced internal electric fields(IEFs),with the former IEF being stronger than the latter,in conjunction with the doped S atom.Density functional theory calculations further unveiled that the intensity of the IEF directly influenced the adsorption of Na+,thereby resulting in the exceptional performances of S-N-CBFs as sodium-ion storage materials.This work uncovers the pivotal role of IEF in regulating the electronic structure of carbon materials and enhancing their Na^(+)storage capabilities,providing valuable insights for the development of more advanced electrode materials.展开更多
The N,S co-doped porous carbon nanofibers were fabricated by the carbonization of[Zn_(2)(tdc)_(2)(MA)]n MOFs/polyacrylonitrile nanofibers composite,which was produced by the electrospinning technology.The electrochemi...The N,S co-doped porous carbon nanofibers were fabricated by the carbonization of[Zn_(2)(tdc)_(2)(MA)]n MOFs/polyacrylonitrile nanofibers composite,which was produced by the electrospinning technology.The electrochemical results show that the N,S co-doped porous carbon nanofibers can achieve capacity of 201.2 mAh·g^(-1)at the current density of 0.05 A·g^(-1).Furthermore,the reversible capacity still has 161.3 mAh·g^(-1)even at a high current density of 1 A·g^(-1)after 600 cycles.The superior electrochemical performance shows that the N,S co-doped porous carbon nanofibers electrode material can be used as an ideal anode material for sodium-ion batteries.展开更多
In near-field communication(NFC)antennas,soft magnetic ferrites are usually applied as a substrate to reduce eddy current loss and increase magnetic field coupling.For this purpose,the applied ferrites are required to...In near-field communication(NFC)antennas,soft magnetic ferrites are usually applied as a substrate to reduce eddy current loss and increase magnetic field coupling.For this purpose,the applied ferrites are required to have high permeability and saturation magnetization together with low magnetic loss and dielectric loss.However,for most soft magnetic ferrites,it is difficult to meet all the requirements.Herein novel Ni-Zn ferrite ceramics co-doped by Ho^(3+)and Co^(2+)ions with chemical formula Ni_(0.5-x)Zn_(0.5)Ho_(0.02)Co_(x)Fe_(1.98)O_(4)(x=0-0.2)were designed and prepared to balance these needs on the basis of molten salt synthesis with metal nitrates as raw materials and potassium hydroxide(KOH)as the precipitation agent and molten salt precursor.After the substitution of Ho^(3+),the saturation magnetization and initial permeability decrease,but with further doping of Co^(2+),the saturation magnetization gradually increases,while the initial permeability continues to decrease.When x=0.1,the sample will have the lowest dielectric constant,magnetic and dielectric loss,as well as the highest Curie temperature(305℃).Moreover,the acquired Ni-Zn ferrites have been applied simulatively in NFC antennas,revealing that the device manufactured with the optimal Ni_(0.4)Zn_(0.5)Ho_(0.02)Co_(0.1)Fe_(1.98)O_(4)ferrite ceramics would have significantly improved performance at 13.56 MHz with low leakage and long transmit distance of magnetic field.Therefore,the Ni_(0.4)Zn_(0.5)Ho_(0.02)Co_(0.1)Fe_(1.98)O_(4)ferrite ceramics would be a good candidate for NFC antenna substrates.展开更多
Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.Howev...Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.展开更多
In this work,we report a novel one-dimensional metal-organic framework(MOF)templated for the synthesis of transition metal sulfides with excellent oxygen evolution reaction(OER)performance via a self-sulfidation proce...In this work,we report a novel one-dimensional metal-organic framework(MOF)templated for the synthesis of transition metal sulfides with excellent oxygen evolution reaction(OER)performance via a self-sulfidation process,eliminating the need for additional sulfur sources.After pyrolysis,MOFs containing Co ions as the metal nodes and 1-phenyl-5-mercaptotetrazole(PMTA)as the ligand were transformed to Co_(9)S_(8)nanoparticles,which were encapsulated in a nitrogen and sulfur dual-doped carbon(Co_(9)S_(8)@NSC)matrix.Additionally,PMTA,as a ligand,possesses the unique advantage of forming porous coordination polymers with a wide range of metals(e.g.,Fe,Ni,and Cu),enabling the versatile synthesis of transition metal sulfide electrocatalysts.Consequently,when served as the electrocatalyst for OER,the N,S co-doped Co_(9)S_(8)@NSC porous nanotubes exhibited excellent OER performance with the overpotential of only 248 mV at 10 mA cm^(−2)and long-term stability.These works provide new insights and inspiration for the rational design and development of non-precious metal-based sulfides with practical potential applications.展开更多
Magnetically separated and N, S co-doped mesoporous carbon microspheres (NIS-MCMs/Fe304) are fabricated by encapsulating Si02 nanoparticles within N, S-containing polymer microspheres which were prepared using resor...Magnetically separated and N, S co-doped mesoporous carbon microspheres (NIS-MCMs/Fe304) are fabricated by encapsulating Si02 nanoparticles within N, S-containing polymer microspheres which were prepared using resorcinol/formaldehyde as the carbon source and cysteine as the nitrogen and sulfur co-precursors, followed by the carbonization process, silica template removal, and the introduction of Fe3O4 into the carbon mesopores. N/S-MCMs/Fe3O4 exhibits an enhanced Hg2+ adsorption capacity of 74.5 rag/g, and the adsorbent can be conveniently and rapidly separated from wastewater using an external magnetic field. This study opens up new opportunities to synthesize well- developed, carbon-based materials as an adsorbent for potential applications in the removal of mercury ions from wastewater.展开更多
A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanat...A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.展开更多
Silicon(Si)is a promising anode candidate for next-generation lithium-ion batteries(LIBs),but it suffers from poor electronic conductivity and dramatic volume variation during cycling,which poses a critical challenge ...Silicon(Si)is a promising anode candidate for next-generation lithium-ion batteries(LIBs),but it suffers from poor electronic conductivity and dramatic volume variation during cycling,which poses a critical challenge for stable battery operation.To mitigate these issues simultaneously,we propose a"double carbon synergistic encapsulation"strategy,namely thin carbon shell and nitrogen/phosphorus co-doped two-dimensional(2D)carbon sheet dual encapsulate Si nanoparticles(denoted as 2D NPC/C@Si).This double carbon structure can serve as a conductive medium and buffer matrix to accommodate the volume expansion of Si nanoparticles and enable fast electron/ion transport,which promotes the formation of a stable solid electrolyte interphase film during cycling.Through structural advantages,the resulting 2 D NPC/C@Si electrode demonstrates a high reversible capacity of592 mAh·g^(-1) at 0.2 A·g^(-1) with 90.5%excellent capacity retention after 100 cycles,outstanding rate capability(148 mAh·g^(-1) at 8 A·g^(-1)),and superior long-term cycling stability(326 mAh·g^(-1) at 1 A·g^(-1) for 500 cycles,86%capacity retention).Our findings elucidate the development of high-performance Si@C composite anodes for advanced LTBs.展开更多
In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using...In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.展开更多
The as-sintered sinter skin of WC-11Co-0.71Cr3C2-0.06RE cemented carbide with WC+βmicrostructure was analyzed by scanning electron microscope, energy dispersive X-ray spectroscope and X-ray diffractometer. RE repres...The as-sintered sinter skin of WC-11Co-0.71Cr3C2-0.06RE cemented carbide with WC+βmicrostructure was analyzed by scanning electron microscope, energy dispersive X-ray spectroscope and X-ray diffractometer. RE represents La-, Ce-, Pr- and Nd-containing mischmetal, andβis cobalt-based binder phase. It was discovered that La, Ce, Pr and Nd migrated directionally from the alloy to the sinter skin to combine with the impurity elements S and O from the sintering atmosphere during the sintering process. As a result, main dispersed phase RE2S3 and minor RE2O2S were formed in situ on the sinter skin. The mechanisms for the stimulation of the migration activity and the directional migration of RE atoms were discussed in terms of the thermodynamics stability of Cr3C2, solubility characteristic of Cr in Co and the polarization or ionization of RE atoms.展开更多
The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the explorat...The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts.展开更多
The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution rea...The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.展开更多
Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in seconda...Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金Project supported by the Innovation Foundation of Beijing University of Aeronautics and Astronautics for PhD Graduates, China (Grant No. 292122)the Equipment Research Foundation of China (Grant No. 373974)
文摘ZnO thin films co-doped with A1 and Sb with different concentrations and a fixed molar ratio of AlCl3 to SbCl3 at 1:2, are prepared by a sol-gel spin-coating method on glass annealed at 550 ℃ for 2 h in air. The x-ray diffraction results confirm that the ZnO thin films co-doped with Al distortion, and the biaxial stresses are 1.03× 10^8. 3.26× 10^8 and Sb are of wurtzite hexagonal ZnO with a very small 5.23 × 10^8, and 6.97× 10^8 Pa, corresponding to those of the ZnO thin films co-doped with Al and Sb in concentrations of 1.5, 3.0, 4.5, 6.0 at% respectively. The optical properties reveal that the ZnO thin films co-doped with Al and Sb have obviously enhanced transmittance in the visible region. The electrical properties show that ZnO thin film co-doped with Al and Sb in a concentration of 1.5 at% has a lowest resistivity of 2.5 Ω·cm.
基金the University Grants Commission (UGC) for providing BSR fellowship
文摘Undoped and Ni–S co-doped mesoporous TiO2 nano materials were synthesized by using sol–gel method.The characteristic features of as prepared catalyst samples were investigated using various advanced spectroscopic and analytical techniques.The characterization results of the samples revealed that all the samples exhibited anatase phase(XRD),decreasing band gap(2.68 eV)(UV–Vis-DRS),small particle size(9.2 nm)(TEM),high surface area(142.156 m^2·g^-1)(BET),particles with spherical shape and smooth morphology(SEM);there is a frequency shift observed for co-doped sample(FT-IR)and the elemental composition electronic states and position of the doped elements(Ni and S)in the TiO2 lattice analyzed by XPS and EDX.These results supported the photocatalytic degradation of Bismarck Brown Red(BBR)achieved with in 110 min and also exhibited the antibacterial activity on Staphylococcus aureus(MTCC-3160),Pseudomonas fluorescence(MTCC-1688)under visible light irradiation.
文摘Nitrogen and phosphorus co-doped graphene quantum dot-modified Bi5O7 I(NPG/Bi5O7 I)nanorods were fabricated via a simple solvothermal method.The morphology,structure,and optical properties of the as-prepared samples were investigated by X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),and diffused reflectance spectroscopy.The photocatalytic performance was estimated by degrading the broad-spectrum antibiotics tetracycline and enrofloxacin under visible light irradiation.The photodegradation activity of Bi5O7 I improved after its surface was modified with NPGs,which was attributed to an increase in the photogenerated charge transport rate and a decrease in the electron-hole pair recombination efficiency.From the electron spin resonance spectra,XPS valence band data,and free radical trapping experiment results,the main active substances involved in the photocatalytic degradation process were determined to be photogenerated holes and superoxide radicals.A possible photocatalytic degradation mechanism for NPG/Bi5O7 I nanorods was proposed.
基金supported by the Taishan Scholars Program of Shandong Province(tsqn202103051)the Project of Scientific Research in Shihezi University(CXFZ202205)。
文摘This work aims to solve the problems of low reaction activity of Cu-based catalysts and agglomeration of active centers in acetylene hydrochlorination.Cu-based catalysts supported by NAP co-doped activated carbon(AC)with different content(mCu-xNP/AC)were manufactured and applied in the acetylene hydrochlorination reaction.It was found that the doping of carriers N and P induced the transformation of Cu^(2+)to Cu^(+),and the catalytic activity was markedly improved.Under the optimal reaction temperature of 220℃,the gas hourly space velocity(GHSV)of C_(2)H_(2)was 90 h^(-1)and V_(HCl):V_(C_(2)H_(2))was 1.15.The initial activity of the 5%Cu-30 NP/AC catalyst reached 95.59%.Through some characterization methods showed the addition of N and P improved the dispersion of Cu in carbon,which increased the ratio of Cu^+/Cu^(2+).The measurement results confirmed that the chemisorption capacity of mCu-xNP/AC for C_(2)H_(2)decreased slightly,and the chemisorption capacity for HCl increased significantly,which was the reason for the increased activity of the catalyst.The conclusion provides a reference for the development of acetylene hydrochlorination Cu catalyst.
文摘In the present work it is studied the phosphorus-aluminum co-doping effect on the electronic and structural graphene properties using ab initio calculations in the framework of DFT (density functional theory). The doping of graphene with substituent heteroatoms can modify the band structures as well as the electron transfer, improving the electronic performance that could enhance the sensing ability in gas sensor devices. The incorporation of heteroatoms in the graphene monolayer alters the unit cell. The alteration degree depends on the dopant concentration. Furthermore, the electronic properties were modified by opening the gap up to 0.61 eV produced by the combination of phosphorus and aluminum as dopants. The dopant concentration can be controlled, which causes different degrees of semiconductor behavior on the co-doped graphene.
基金financial support by the National Natural Science Foundation of China (Grant: 51333008)Young Teacher Training Program of Sun Yat-sen University (Grant: 17lgpy86)
文摘Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium.
基金the National Natural Science Foundation of China(No.22138013).
文摘Heteroatom doping has emerged as a prevailing strategy to enhance the storage of sodium ions in carbon materials.However,the underlying mechanism governing the performance enhancement remains undisclosed.Herein,we fabricated N/S co-doped carbon beaded fibers(S-N-CBFs),which exhibited glorious rate performance and durableness in Na+storage,showcasing no obvious capacity decay even after 3500 cycles.Furthermore,when used as anodes in sodium-ion capacitors,the S-N-CBFs delivered exceptional results,boasting a high energy density of 225 Wh·kg^(-1),superior power output of 22500 W·kg^(-1),and outstanding cycling stability with a capacity attenuation of merely 0.014%per cycle after 4000 cycles at 2 A·g^(-1).Mechanistic investigations revealed that the incorporation of both pyridinic N and pyrrolic N into the carbon matrix of S-N-CBFs induced internal electric fields(IEFs),with the former IEF being stronger than the latter,in conjunction with the doped S atom.Density functional theory calculations further unveiled that the intensity of the IEF directly influenced the adsorption of Na+,thereby resulting in the exceptional performances of S-N-CBFs as sodium-ion storage materials.This work uncovers the pivotal role of IEF in regulating the electronic structure of carbon materials and enhancing their Na^(+)storage capabilities,providing valuable insights for the development of more advanced electrode materials.
文摘The N,S co-doped porous carbon nanofibers were fabricated by the carbonization of[Zn_(2)(tdc)_(2)(MA)]n MOFs/polyacrylonitrile nanofibers composite,which was produced by the electrospinning technology.The electrochemical results show that the N,S co-doped porous carbon nanofibers can achieve capacity of 201.2 mAh·g^(-1)at the current density of 0.05 A·g^(-1).Furthermore,the reversible capacity still has 161.3 mAh·g^(-1)even at a high current density of 1 A·g^(-1)after 600 cycles.The superior electrochemical performance shows that the N,S co-doped porous carbon nanofibers electrode material can be used as an ideal anode material for sodium-ion batteries.
基金This work was supported by the National Natural Science Foundation of China(Nos.11674035 and 61274015)the Fundamental Research Funds for the Central Universities.
文摘In near-field communication(NFC)antennas,soft magnetic ferrites are usually applied as a substrate to reduce eddy current loss and increase magnetic field coupling.For this purpose,the applied ferrites are required to have high permeability and saturation magnetization together with low magnetic loss and dielectric loss.However,for most soft magnetic ferrites,it is difficult to meet all the requirements.Herein novel Ni-Zn ferrite ceramics co-doped by Ho^(3+)and Co^(2+)ions with chemical formula Ni_(0.5-x)Zn_(0.5)Ho_(0.02)Co_(x)Fe_(1.98)O_(4)(x=0-0.2)were designed and prepared to balance these needs on the basis of molten salt synthesis with metal nitrates as raw materials and potassium hydroxide(KOH)as the precipitation agent and molten salt precursor.After the substitution of Ho^(3+),the saturation magnetization and initial permeability decrease,but with further doping of Co^(2+),the saturation magnetization gradually increases,while the initial permeability continues to decrease.When x=0.1,the sample will have the lowest dielectric constant,magnetic and dielectric loss,as well as the highest Curie temperature(305℃).Moreover,the acquired Ni-Zn ferrites have been applied simulatively in NFC antennas,revealing that the device manufactured with the optimal Ni_(0.4)Zn_(0.5)Ho_(0.02)Co_(0.1)Fe_(1.98)O_(4)ferrite ceramics would have significantly improved performance at 13.56 MHz with low leakage and long transmit distance of magnetic field.Therefore,the Ni_(0.4)Zn_(0.5)Ho_(0.02)Co_(0.1)Fe_(1.98)O_(4)ferrite ceramics would be a good candidate for NFC antenna substrates.
基金supported by the National Natural Science Foundation of China(No.52002320,and 51972267)the China Postdoctoral Science Foundation(No.2022M712574)+3 种基金the Science Foundation of Shaanxi Province(2022GD-TSLD-18,No.2023-JCZD-03)Natural Science Foundation of Shaanxi Province(No.2022GY-372,2021GY-153)Industrial Projects Foundation of Ankang Science and Technology Bureau(No.AK2020-GY02-2)the Platform Construction Projects and Technology Service Teams of Ankang University(No.2021AYPT12 and 2022TD07)。
文摘Sodium-ion batteries(SIBs) and hybrid capacitors(SIHCs) have garnered significant attention in energy storage due to their inherent advantages,including high energy density,cost-effectiveness,and enhanced safety.However,developing high-performance anode materials to improve sodium storage performa nce still remains a major challenge.Here,a facile one-pot method has been developed to fabricate a hybrid of MoSeTe nanosheets implanted within the N,F co-doped honeycomb carbon skeleton(MoSeTe/N,F@C).Experimental results demonstrate that the incorporation of large-sized Te atoms into MoSeTe nanosheets enlarges the layer spacing and creates abundant anion vacancies,which effectively facilitate the insertion/extraction of Na^(+) and provide numerous ion adsorption sites for rapid surface capacitive behavior.Additionally,the heteroatoms N,F co-doped honeycomb carbon skeleton with a highly conductive network can restrain the volume expansion and boost reaction kinetics within the electrode.As anticipated,the MoSeTe/N,F@C anode exhibits high reversible capacities along with exceptional cycle stability.When coupled with Na_(3)V_(2)(PO_(4))_(3)@C(NVPF@C) to form SIB full cells,the anode delivers a reversible specific capacity of 126 mA h g^(-1) after 100 cycles at 0.1 A g^(-1).Furthermore,when combined with AC to form SIHC full cells,the anode demonstrates excellent cycling stability with a reversible specific capacity of50 mA h g^(-1) keeping over 3700 cycles at 1.0 A g^(-1).In situ XRD,ex situ TEM characterization,and theoretical calculations(DFT) further confirm the reversibility of sodium storage in MoSeTe/N,F@C anode materials during electrochemical reactions,highlighting their potential for widespread practical application.This work provides new insights into the promising utilization of advanced transition metal dichalcogenides as anode materials for Na^(+)-based energy storage devices.
基金supported by the National Natural Science Foundation of China(21701059,51902140 and 52102100)the Natural Science Foundation of Jiangsu Province for Youths(BK20170571).
文摘In this work,we report a novel one-dimensional metal-organic framework(MOF)templated for the synthesis of transition metal sulfides with excellent oxygen evolution reaction(OER)performance via a self-sulfidation process,eliminating the need for additional sulfur sources.After pyrolysis,MOFs containing Co ions as the metal nodes and 1-phenyl-5-mercaptotetrazole(PMTA)as the ligand were transformed to Co_(9)S_(8)nanoparticles,which were encapsulated in a nitrogen and sulfur dual-doped carbon(Co_(9)S_(8)@NSC)matrix.Additionally,PMTA,as a ligand,possesses the unique advantage of forming porous coordination polymers with a wide range of metals(e.g.,Fe,Ni,and Cu),enabling the versatile synthesis of transition metal sulfide electrocatalysts.Consequently,when served as the electrocatalyst for OER,the N,S co-doped Co_(9)S_(8)@NSC porous nanotubes exhibited excellent OER performance with the overpotential of only 248 mV at 10 mA cm^(−2)and long-term stability.These works provide new insights and inspiration for the rational design and development of non-precious metal-based sulfides with practical potential applications.
基金financially supported by the National Natural Science Foundation of China (Nos. 21207099, 21273162, and 21473122)the Science and Technology Commission of Shanghai Municipality, China (No. 14DZ2261100)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Large Equipment Test Foundation of Tongji University
文摘Magnetically separated and N, S co-doped mesoporous carbon microspheres (NIS-MCMs/Fe304) are fabricated by encapsulating Si02 nanoparticles within N, S-containing polymer microspheres which were prepared using resorcinol/formaldehyde as the carbon source and cysteine as the nitrogen and sulfur co-precursors, followed by the carbonization process, silica template removal, and the introduction of Fe3O4 into the carbon mesopores. N/S-MCMs/Fe3O4 exhibits an enhanced Hg2+ adsorption capacity of 74.5 rag/g, and the adsorbent can be conveniently and rapidly separated from wastewater using an external magnetic field. This study opens up new opportunities to synthesize well- developed, carbon-based materials as an adsorbent for potential applications in the removal of mercury ions from wastewater.
文摘A series of photocatalysts of un-doped, single-doped and co-doped nanometer titanium diox- ide (TiO2) have been successfully prepared by template method using Fe(NO3)3.9H2O, La(NO3)3.6H2O, and tetrabutyl titanate as precursors and glucan as template. Scanning electron microscopy, X-ray diffraction, and N2 adsorption-desorption measurement were employed to characterize the morphology, crystal structure and surface structure of the samples. The photo-absorbance of the obtained catalysts was measured by UV-Vis absorption spectroscopy, and the photocatalytic activities of the prepared samples under UV and visible light were estimated by measuring the degradation rate of methyl orange in an aqueous solution. The characterizations indicated that the prepared photocatalysts consisted of anatase phase and possessed high surface area of ca. 163-176 m2/g. It was shown that the Fe and La co-doped nano-TiO2 could be activated by visible light and could thus be used as an effective catalyst in photo-oxidation reactions. The synergistic effect of Fe and La co-doping played an important role in improving the photocatalytic activity. In addition, the possibility of cyclic usage of co-doped nano-TiO2 was also confirmed, the photocatalytic activity of codoped nano-TiO2 remained above 89.6% of the fresh sample after being used four times.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52072323,21805278 and 51872098)the Leading Project Foundation of Science Department of Fujian Province(No.2018H0034)+2 种基金the“Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen Universitythe Opening Project of National Joint Engineering Research Center for Abrasion Control and Molding of Metal MaterialsHenan Key Laboratory of High-temperature Structural and Functional Materials,Henan University of Science and Technology(No.HKDNM2019013)。
文摘Silicon(Si)is a promising anode candidate for next-generation lithium-ion batteries(LIBs),but it suffers from poor electronic conductivity and dramatic volume variation during cycling,which poses a critical challenge for stable battery operation.To mitigate these issues simultaneously,we propose a"double carbon synergistic encapsulation"strategy,namely thin carbon shell and nitrogen/phosphorus co-doped two-dimensional(2D)carbon sheet dual encapsulate Si nanoparticles(denoted as 2D NPC/C@Si).This double carbon structure can serve as a conductive medium and buffer matrix to accommodate the volume expansion of Si nanoparticles and enable fast electron/ion transport,which promotes the formation of a stable solid electrolyte interphase film during cycling.Through structural advantages,the resulting 2 D NPC/C@Si electrode demonstrates a high reversible capacity of592 mAh·g^(-1) at 0.2 A·g^(-1) with 90.5%excellent capacity retention after 100 cycles,outstanding rate capability(148 mAh·g^(-1) at 8 A·g^(-1)),and superior long-term cycling stability(326 mAh·g^(-1) at 1 A·g^(-1) for 500 cycles,86%capacity retention).Our findings elucidate the development of high-performance Si@C composite anodes for advanced LTBs.
基金This work was supported by the National Natural Sci- ence Foundation of China (No.41373127) and the Liaoning Provincial Natural Science Foundation of China (No.2013020121).
文摘In order to improve the photocatalytic performance of mesoporous titania under visible light, a series of photocatalysts of S and Ag co-doped mesoporous titania have been successfully prepared by template method using thiourea, AgNO3 and tetrabutyl titanate as precursors and Pluronic P123 (EO20PO70EO20) as template. Scanning electron microscopy (SEM), X-ray diffraction (XRD), nitrogen adsorption-desorption measurements, and UV-visible spectroscopy (UV-Vis) were employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The microcrystal of the photocatalysts consisted of anatase phase and was approximately present in the form of spherical particle. The photocatalytic performance was studied by photodegradation methyl orange (MO) in water under UV and visible light irradiation. The calcination temperature and the doping content influenced the photoactivity. In addition, the possibility of cyclic usage of co-doped mesoporous titania was also confirmed, the photocatalytic activity of mesoporous titania remained above 89% of that of the fresh sample after being used four times. It was shown that the co-doped mesoporous titania could be activated by visible light and could thus be potentially applied for the treatment of water contaminated by organic pollutants. The synergistic effect of sulfur and silver co-doping played an important role in improving the photocatalytic activity.
基金Project(51074189)supported by the National Natural Science Foundation of ChinaProject(2012ZX04003–021)supported by the National Science&Technology Special Foundation of ChinaProject(Y2012–010)supported by the Nonferrous Metals Research Foundation from Hunan Nonferrous Metals Holding Group Co.,Ltd.–CSU,China
文摘The as-sintered sinter skin of WC-11Co-0.71Cr3C2-0.06RE cemented carbide with WC+βmicrostructure was analyzed by scanning electron microscope, energy dispersive X-ray spectroscope and X-ray diffractometer. RE represents La-, Ce-, Pr- and Nd-containing mischmetal, andβis cobalt-based binder phase. It was discovered that La, Ce, Pr and Nd migrated directionally from the alloy to the sinter skin to combine with the impurity elements S and O from the sintering atmosphere during the sintering process. As a result, main dispersed phase RE2S3 and minor RE2O2S were formed in situ on the sinter skin. The mechanisms for the stimulation of the migration activity and the directional migration of RE atoms were discussed in terms of the thermodynamics stability of Cr3C2, solubility characteristic of Cr in Co and the polarization or ionization of RE atoms.
基金supported financially by the National Natural Science Foundation of China (No. 21905271)Liaoning Natural Science Foundation (No. 20180510029)the Dalian National Laboratory for Clean Energy (DNL), DNL Cooperation Fund, Chinese Academy of Sciences (No. DNL180402)。
文摘The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts.
基金Collaborative Innovation Center of Suzhou Nano Science and TechnologyNational Natural Science Foundation of China,Grant/Award Numbers:21773163,22271203+3 种基金EPSRC for an Overseas Travel Grant,Grant/Award Number:EP/R023816/1State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry,Grant/Award Number:KF2021005Priority Academic Program Development of Jiangsu Higher Education InstitutionsProject of Scientific and Technologic Infrastructure of Suzhou,Grant/Award Number:SZS201905。
文摘The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent issue.Herein,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is developed.The multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline media.The optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery system.This work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.
基金financially supported by the Shenzhen Science and Technology Program(JCYJ20220530141012028),ChinaThe National Natural Science Foundation of China(22005178),China+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01),ChianThe fellowship of China Postdoctoral Science Foundation(2022M722333),Chianthe Jiangsu Funding Program for Excellent Postdoctoral Talent,Chian。
文摘Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.