Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses...Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.展开更多
Highly supersaturated nanocrystalline fcc Fe60Cu40 alloy has been prepared by mechanical alloying of elemental powders. The phase transformation is monitored by X-ray diffraction (XRD),Mossbauer spectroscopy and exten...Highly supersaturated nanocrystalline fcc Fe60Cu40 alloy has been prepared by mechanical alloying of elemental powders. The phase transformation is monitored by X-ray diffraction (XRD),Mossbauer spectroscopy and extended X-ray absorption fine structure (EXAFS). The powder obtained after milling is of single fcc structure with grain size of nanometer order. The Mossbauer spectra of the milled powder can be fitted by two subspectra whose hyperfine magnetic fields are 16 MA/m and 20 MA/m while that of pure Fe disappeared. EXAFS results show that the radial structure function (RSF) of Fe K-edge changed drastically and finally became similar to that of reference Cu K-edge, while that of Cu K-edge nearly keeps unchanged in the process of milling. These imply that bcc Fe really transforms to fcc structure and alloying between Fe and Cu occurs truly on an atomic scale. EXAFS results indicate that iron atoms tend to segregate at the boundaries and Cu atoms are rich in the fcc lattice. Annealing experiments show that the Fe atoms at the interfaces are easy to cluster to α-Fe at a lower temperature, whereas the iron atoms in the lattice will form γ-Fe first at temperature above 350℃, and then transform to bcc Fe展开更多
Structural and magnetic properties are investigated for Fe1-xMnxV2O4 (0≤ x ≤ 1) spinels. As orbital-active Fe^2+ is substituted with Mn^2+, the cubie-to-tetragonM transition TsI and the tetragonal-to-orthorhombi...Structural and magnetic properties are investigated for Fe1-xMnxV2O4 (0≤ x ≤ 1) spinels. As orbital-active Fe^2+ is substituted with Mn^2+, the cubie-to-tetragonM transition TsI and the tetragonal-to-orthorhombic transition Ts2 gradually decrease. These structural transitions originate from the Fe^2+ ferro-orbital order (F-OO). Below Yafet-Kittel (YK) magnetic transition TN2, V^3+ orbital order (V-OO) plays an important role on global structure. Here x = 0.6 is a critical point. Fe^2+ F-OO and V^3+ F-OO coexist for 0 ≤ x ≤ 0.5. For x≥ 0.6, the orbital pattern of V^3+ is antiferro (AF)-00, and Fe^2+ F-OO disappears. Structural transition Ts3, accompanied by YK magnetic transition TN2, decreases initially, and then increases at x = 0.6. A scenario for the complex phase diagram arising from the cooperation or competition of Fe^2+ and V^3+ orbitals is proposed.展开更多
Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high ca...Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high catalyst loadings required. In the present work, mesoporous Fe/N/C was syn- thesized through heat treatment of K]600 carbon black coated with poly-2-aminobenzimidazole and FeC13. The as-prepared Fe/N/C possesses a unique hollow-shell structure that contains a buffer zone allowing both water formation and vaporization, and also facilitates the mass transfer of gas- eous oxygen. This catalyst generated an oxygen reduction reaction activiW of 9.21 A/g in conjunc- tion with a peak power density of 0.71 W/cm2.展开更多
The structure and magnetic properties of Fe76.5Si13.5B9Cu1 alloys with a nanocrystalline (NC) bcc Fe(Si) phase trom about 23 to 46 nm in diameter, which were first formed into amorphous ribbons and then annealed at va...The structure and magnetic properties of Fe76.5Si13.5B9Cu1 alloys with a nanocrystalline (NC) bcc Fe(Si) phase trom about 23 to 46 nm in diameter, which were first formed into amorphous ribbons and then annealed at various temperatures between 703 and 773 K, have been investigated. At annealing temperatures from 703 to 748 K, the single NC bcc(Si) phase is obtained in the crystallized alloys. The grain size and the Si-content in the NC bcc Fe(Si) phase for the alloys annealed at different temperatures are presented. The soft magnetic properties and the saturation magnetostriction for the alloys with the NC bcc Fe(Si) phase are also measured. The results show that, the saturation magnetizotion and the permeability are improved for the alloys with only the NC bcc Fe(Si) phase and become better with decreasing of the NC bcc phase size, and the saturation magnetostriction declines for the alloys with increasing Si-content in the NC bcc Fe(Si) phase.展开更多
The purpose of this study is to explore the adsorption performance of meso-2,3-dimercaptosuccinic acid(DMSA)modified Fe3O4@SiO2 magnetic nanocomposite(Fe3O4@SiO2@DMSA)for Pb2+ions removal from aqueous solutions.The ef...The purpose of this study is to explore the adsorption performance of meso-2,3-dimercaptosuccinic acid(DMSA)modified Fe3O4@SiO2 magnetic nanocomposite(Fe3O4@SiO2@DMSA)for Pb2+ions removal from aqueous solutions.The effects of solution pH,initial concentration of Pb2+ions,contact time,and temperature on the amount of Pb2+adsorbed were investigated.Adsorption isotherms,adsorption kinetics,and thermodynamic analysis were also studied.The results showed that the maximum adsorption capacity of the Fe3O4@SiO2@DMSA composite is 50.5 mg/g at 298 K,which is higher than that of Fe3O4 and Fe3O4@SiO2 magnetic nanoparticles.The adsorption process agreed well with Langmuir adsorption isotherm models and pseudo second-order kinetics.The thermodynamic analysis revealed that the adsorption was spontaneous,endothermic and energetically driven in nature.展开更多
Reaction of ferrocenoyl chloride with [Et;NH] [(μ-CO)(μ-RS) Fe;=(CO);] complexes gave bridging ferrocenoyl complexes(μ-FcCO)(μ-RS)Fe;(CO);(Fc=ferrocenyl, R=Et, i-Pr, n-Bu, t-Bu, Ph).The structures of all...Reaction of ferrocenoyl chloride with [Et;NH] [(μ-CO)(μ-RS) Fe;=(CO);] complexes gave bridging ferrocenoyl complexes(μ-FcCO)(μ-RS)Fe;(CO);(Fc=ferrocenyl, R=Et, i-Pr, n-Bu, t-Bu, Ph).The structures of all new complexes were characterised by;HNMR, IR and MS.展开更多
The microwave radiation method was introduced to prepare the Fe_2O_3/SO solid superacid.Its structure and properties were investigated by means of X-ray diffraction and infrared spectrum analyses as well as measuremen...The microwave radiation method was introduced to prepare the Fe_2O_3/SO solid superacid.Its structure and properties were investigated by means of X-ray diffraction and infrared spectrum analyses as well as measurement of magnetic susceptibility and rate of esterification. The structure of the superacids prepared in microwave field can be crystalline or non-crystalline, the latter has not been reported yet in literatures. Comparing with the traditional superacid, the non-crystalline Fe2O3/SO superacid prepared in microwave field has the highest magnetic susceptibility and catalytic activity. The di-coordination of Fe2O3 and SO and the S=O bi-bond were reinforced by microwave radiation, which is favorable for increasing the acid intensity of the Fe2O3/SO catalyst展开更多
Many researchers have studied on perovskite oxide for its unique structure.Perovskite oxides,ABO3-δ,with different A and B metals have shown wide applications in many fields,in particular solid oxide electrolysers.Sr...Many researchers have studied on perovskite oxide for its unique structure.Perovskite oxides,ABO3-δ,with different A and B metals have shown wide applications in many fields,in particular solid oxide electrolysers.SrFeO3-δ,typical perovskite oxides,in which iron is the mixed-valence cation with the capacity to change the chemical valence,have a wide range of oxygen nonstoichiometry.In this study,Sr(0.9)Fe(0.9)Zr(0.1)O3-δ(SFZO) is synthesized and then treated in 5%H2/Ar and air at high temperature,exhibiting excellent redox stability.Redox-stable structure,oxygen vacancy and electrical properties of SFZO are investigated.Steam electrolysis is then performed with SFZO cathode under 5%H2O/5%H2/Ar and 5%H2O/Ar atmospheres,respectively.The present results indicate that the SFZO is a novel promising cathode material for solid oxide steam electrolyser.展开更多
A structure transition of Fe2O3 nanocrystal was studied by using DTA and TG thermal analysis and X-ray diffraction method. We found that size increase of the nanocrystals is larger after the structure transition than ...A structure transition of Fe2O3 nanocrystal was studied by using DTA and TG thermal analysis and X-ray diffraction method. We found that size increase of the nanocrystals is larger after the structure transition than that before the transition. It means that the structure transition is beneficial on growth of nanocrystals展开更多
Fe/C multilayer thin films were deposited by magnetron sputtering. Small angle X-ray diffraction measurements show very well periodicity of the samples. The modulation period determined from a modified Bragg equation ...Fe/C multilayer thin films were deposited by magnetron sputtering. Small angle X-ray diffraction measurements show very well periodicity of the samples. The modulation period determined from a modified Bragg equation agrees well with that determined from deposition rate. The interfacial roughness parameter ξof several samples calculated by X-ray diffraction is between 3.5(?) and 5.6(?).展开更多
The Co content dependence of crystal structure and specific magnetization of Fe1-xCox-SiO2granular solid prepared by the sol-gel method have been studied. It is found that the crystal structure, Iattice parameter and ...The Co content dependence of crystal structure and specific magnetization of Fe1-xCox-SiO2granular solid prepared by the sol-gel method have been studied. It is found that the crystal structure, Iattice parameter and specific magnetization of the FeCo alloy particles depend on the Co content.展开更多
The crystal structure of the title complex salt has been determined by single-crystal X-ray structure analysis. The crystal data are as follows; Monoclinic, P21/c, a=15.6480(10)A,b=16.7870(10)A, c=10.347(2)A, β=90.79...The crystal structure of the title complex salt has been determined by single-crystal X-ray structure analysis. The crystal data are as follows; Monoclinic, P21/c, a=15.6480(10)A,b=16.7870(10)A, c=10.347(2)A, β=90.790(10), V=2717.7(6)A3, Z=3, and R=0.0333 for 4789 unique reflections. The complex anion has a pseudo-octahedral structure distorted more than the CrⅢand CoⅢ analogs, in which cach iminodiacetato ligand (ida2-) is coordinated in a facial fashion with the two N atoms in a cis configuration, resulting in an unsyin-fac structure.展开更多
The controlled synthesis of hollow magnetite (Fe3O4) nanospheres of varying sizes and structures was successfully obtained via a facile solvothermal process and varying cooling processes. The Fe3O4 nanospheres were ...The controlled synthesis of hollow magnetite (Fe3O4) nanospheres of varying sizes and structures was successfully obtained via a facile solvothermal process and varying cooling processes. The Fe3O4 nanospheres were characterized by X-ray diffraction, transmission electron microscopy, scanning elec- tron microscopy, and superconducting quantum interference device magnetometry. The diameters of the as-synthesized nanospheres were controlled at around 500-700 nm by simply changing the cool- ing rate, which had an obvious influence on the morphology and magnetic properties of these Fe3O4 nanospheres. While a low cooling rate triggered the formation and extension of the cracks present in the Fe3O4 nanospheres, a sudden drop of temperature tended to favor multi-site nucleation of the crystals as well as the formation of compact and smooth hollow nanospheres with superior crystallinity and high saturation magnetization. The growth mechanism of hollow magnetite oxide nanospheres was proposed and the correlation between the structure and the magnetic properties of the hollow nanospheres was discussed, which promises the potential of the hollow nanospheres in various applications such as drug delivery and cell separation.展开更多
Methylcyclohexane(MCH)serves as an ideal hydrogen carrier in hydrogen storage and transportation process.In the continuous production of hydrogen from MCH dehydrogenation,the rational design of energy-efficient cataly...Methylcyclohexane(MCH)serves as an ideal hydrogen carrier in hydrogen storage and transportation process.In the continuous production of hydrogen from MCH dehydrogenation,the rational design of energy-efficient catalytic way with good performance remains an enormous challenge.Herein,an internal electric heating(IEH)assisted mode was designed and proposed by the directly electrical-driven catalyst using the resistive heating effect.The Pt/Al2O_(3)on Fe foam(Pt/Al2O_(3)/FF)with unique threedimensional network structure was constructed.The catalysts were studied in a comprehensive way including X-ray diffraction(XRD),scanning electron microscopy(SEM)-mapping,in situ extended X-ray absorption fine structure(EXAFS),and in situ COFourier transform infrared(FTIR)measurements.It was found that the hydrogen evolution rate in IEH mode can reach up to above 2060 mmol·gPt^(−1)·min^(−1),which is 2–5 times higher than that of reported Pt based catalysts under similar reaction conditions in conventional heating(CH)mode.In combination with measurements from high-resolution infrared thermometer,the equations of heat transfer rate,and reaction heat analysis results,the Pt/Al2O_(3)/FF not only has high mass and heat transfer ability to promote catalytic performance,but also behaves as the heating component with a low thermal resistance and heat capacity offering a fast temperature response in IEH mode.In addition,the chemical adsorption and activation of MCH molecules can be efficiently facilitated by IEH mode,proved by the operando MCH-FTIR results.Therefore,the as-developed IEH mode can efficiently reduce the heat and mass transfer limitations and prominently boost the dehydrogenation performance,which has a broad application potential in hydrogen storage and other catalytic reaction processes.展开更多
基金funding from the Hellenic Foundation for Research and Innovation(HFRI)under grant agreement No 3655.
文摘Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.
文摘Highly supersaturated nanocrystalline fcc Fe60Cu40 alloy has been prepared by mechanical alloying of elemental powders. The phase transformation is monitored by X-ray diffraction (XRD),Mossbauer spectroscopy and extended X-ray absorption fine structure (EXAFS). The powder obtained after milling is of single fcc structure with grain size of nanometer order. The Mossbauer spectra of the milled powder can be fitted by two subspectra whose hyperfine magnetic fields are 16 MA/m and 20 MA/m while that of pure Fe disappeared. EXAFS results show that the radial structure function (RSF) of Fe K-edge changed drastically and finally became similar to that of reference Cu K-edge, while that of Cu K-edge nearly keeps unchanged in the process of milling. These imply that bcc Fe really transforms to fcc structure and alloying between Fe and Cu occurs truly on an atomic scale. EXAFS results indicate that iron atoms tend to segregate at the boundaries and Cu atoms are rich in the fcc lattice. Annealing experiments show that the Fe atoms at the interfaces are easy to cluster to α-Fe at a lower temperature, whereas the iron atoms in the lattice will form γ-Fe first at temperature above 350℃, and then transform to bcc Fe
基金Supported by the National Basic Research Program of China under Grant Nos 2011CB921904 and 2012CB927402the National Natural Science Foundation of China under Grant Nos 11074142 and 11021464+1 种基金the Key Project of Chinese Ministry of Education under Grant No 309003the Tsinghua TNList Cross-discipline Foundation
文摘Structural and magnetic properties are investigated for Fe1-xMnxV2O4 (0≤ x ≤ 1) spinels. As orbital-active Fe^2+ is substituted with Mn^2+, the cubie-to-tetragonM transition TsI and the tetragonal-to-orthorhombic transition Ts2 gradually decrease. These structural transitions originate from the Fe^2+ ferro-orbital order (F-OO). Below Yafet-Kittel (YK) magnetic transition TN2, V^3+ orbital order (V-OO) plays an important role on global structure. Here x = 0.6 is a critical point. Fe^2+ F-OO and V^3+ F-OO coexist for 0 ≤ x ≤ 0.5. For x≥ 0.6, the orbital pattern of V^3+ is antiferro (AF)-00, and Fe^2+ F-OO disappears. Structural transition Ts3, accompanied by YK magnetic transition TN2, decreases initially, and then increases at x = 0.6. A scenario for the complex phase diagram arising from the cooperation or competition of Fe^2+ and V^3+ orbitals is proposed.
基金supported by the National Basic Research Program of Chain(973 Program,2015CB932300)the National Natural Science Foundation of China(21373175,21321062,21361140374)Fundamental Research Funds for the Central Universities(20720150109)
文摘Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high catalyst loadings required. In the present work, mesoporous Fe/N/C was syn- thesized through heat treatment of K]600 carbon black coated with poly-2-aminobenzimidazole and FeC13. The as-prepared Fe/N/C possesses a unique hollow-shell structure that contains a buffer zone allowing both water formation and vaporization, and also facilitates the mass transfer of gas- eous oxygen. This catalyst generated an oxygen reduction reaction activiW of 9.21 A/g in conjunc- tion with a peak power density of 0.71 W/cm2.
文摘The structure and magnetic properties of Fe76.5Si13.5B9Cu1 alloys with a nanocrystalline (NC) bcc Fe(Si) phase trom about 23 to 46 nm in diameter, which were first formed into amorphous ribbons and then annealed at various temperatures between 703 and 773 K, have been investigated. At annealing temperatures from 703 to 748 K, the single NC bcc(Si) phase is obtained in the crystallized alloys. The grain size and the Si-content in the NC bcc Fe(Si) phase for the alloys annealed at different temperatures are presented. The soft magnetic properties and the saturation magnetostriction for the alloys with the NC bcc Fe(Si) phase are also measured. The results show that, the saturation magnetizotion and the permeability are improved for the alloys with only the NC bcc Fe(Si) phase and become better with decreasing of the NC bcc phase size, and the saturation magnetostriction declines for the alloys with increasing Si-content in the NC bcc Fe(Si) phase.
基金Project(2013DFA51290)supported by International S&T Cooperation Program of China
文摘The purpose of this study is to explore the adsorption performance of meso-2,3-dimercaptosuccinic acid(DMSA)modified Fe3O4@SiO2 magnetic nanocomposite(Fe3O4@SiO2@DMSA)for Pb2+ions removal from aqueous solutions.The effects of solution pH,initial concentration of Pb2+ions,contact time,and temperature on the amount of Pb2+adsorbed were investigated.Adsorption isotherms,adsorption kinetics,and thermodynamic analysis were also studied.The results showed that the maximum adsorption capacity of the Fe3O4@SiO2@DMSA composite is 50.5 mg/g at 298 K,which is higher than that of Fe3O4 and Fe3O4@SiO2 magnetic nanoparticles.The adsorption process agreed well with Langmuir adsorption isotherm models and pseudo second-order kinetics.The thermodynamic analysis revealed that the adsorption was spontaneous,endothermic and energetically driven in nature.
基金The project was supported by Youth Science Foundation of Shandong University
文摘Reaction of ferrocenoyl chloride with [Et;NH] [(μ-CO)(μ-RS) Fe;=(CO);] complexes gave bridging ferrocenoyl complexes(μ-FcCO)(μ-RS)Fe;(CO);(Fc=ferrocenyl, R=Et, i-Pr, n-Bu, t-Bu, Ph).The structures of all new complexes were characterised by;HNMR, IR and MS.
文摘The microwave radiation method was introduced to prepare the Fe_2O_3/SO solid superacid.Its structure and properties were investigated by means of X-ray diffraction and infrared spectrum analyses as well as measurement of magnetic susceptibility and rate of esterification. The structure of the superacids prepared in microwave field can be crystalline or non-crystalline, the latter has not been reported yet in literatures. Comparing with the traditional superacid, the non-crystalline Fe2O3/SO superacid prepared in microwave field has the highest magnetic susceptibility and catalytic activity. The di-coordination of Fe2O3 and SO and the S=O bi-bond were reinforced by microwave radiation, which is favorable for increasing the acid intensity of the Fe2O3/SO catalyst
基金Supported by the National Natural Science Foundation of China(91545123)and the Natural Science Foundation of Fujian Province(2016J01275)
文摘Many researchers have studied on perovskite oxide for its unique structure.Perovskite oxides,ABO3-δ,with different A and B metals have shown wide applications in many fields,in particular solid oxide electrolysers.SrFeO3-δ,typical perovskite oxides,in which iron is the mixed-valence cation with the capacity to change the chemical valence,have a wide range of oxygen nonstoichiometry.In this study,Sr(0.9)Fe(0.9)Zr(0.1)O3-δ(SFZO) is synthesized and then treated in 5%H2/Ar and air at high temperature,exhibiting excellent redox stability.Redox-stable structure,oxygen vacancy and electrical properties of SFZO are investigated.Steam electrolysis is then performed with SFZO cathode under 5%H2O/5%H2/Ar and 5%H2O/Ar atmospheres,respectively.The present results indicate that the SFZO is a novel promising cathode material for solid oxide steam electrolyser.
文摘A structure transition of Fe2O3 nanocrystal was studied by using DTA and TG thermal analysis and X-ray diffraction method. We found that size increase of the nanocrystals is larger after the structure transition than that before the transition. It means that the structure transition is beneficial on growth of nanocrystals
文摘Fe/C multilayer thin films were deposited by magnetron sputtering. Small angle X-ray diffraction measurements show very well periodicity of the samples. The modulation period determined from a modified Bragg equation agrees well with that determined from deposition rate. The interfacial roughness parameter ξof several samples calculated by X-ray diffraction is between 3.5(?) and 5.6(?).
文摘The Co content dependence of crystal structure and specific magnetization of Fe1-xCox-SiO2granular solid prepared by the sol-gel method have been studied. It is found that the crystal structure, Iattice parameter and specific magnetization of the FeCo alloy particles depend on the Co content.
文摘The crystal structure of the title complex salt has been determined by single-crystal X-ray structure analysis. The crystal data are as follows; Monoclinic, P21/c, a=15.6480(10)A,b=16.7870(10)A, c=10.347(2)A, β=90.790(10), V=2717.7(6)A3, Z=3, and R=0.0333 for 4789 unique reflections. The complex anion has a pseudo-octahedral structure distorted more than the CrⅢand CoⅢ analogs, in which cach iminodiacetato ligand (ida2-) is coordinated in a facial fashion with the two N atoms in a cis configuration, resulting in an unsyin-fac structure.
文摘The controlled synthesis of hollow magnetite (Fe3O4) nanospheres of varying sizes and structures was successfully obtained via a facile solvothermal process and varying cooling processes. The Fe3O4 nanospheres were characterized by X-ray diffraction, transmission electron microscopy, scanning elec- tron microscopy, and superconducting quantum interference device magnetometry. The diameters of the as-synthesized nanospheres were controlled at around 500-700 nm by simply changing the cool- ing rate, which had an obvious influence on the morphology and magnetic properties of these Fe3O4 nanospheres. While a low cooling rate triggered the formation and extension of the cracks present in the Fe3O4 nanospheres, a sudden drop of temperature tended to favor multi-site nucleation of the crystals as well as the formation of compact and smooth hollow nanospheres with superior crystallinity and high saturation magnetization. The growth mechanism of hollow magnetite oxide nanospheres was proposed and the correlation between the structure and the magnetic properties of the hollow nanospheres was discussed, which promises the potential of the hollow nanospheres in various applications such as drug delivery and cell separation.
基金the National Natural Science Foundation of China(Nos.22225807,21961132026,21878331,22021004,and 22109177)the National Key Research and Development Program(Nos.2020YFA0210903 and 2021YFA1501304)+4 种基金the PetroChina research institute of petroleum processing program(Nos.PRIKY21057 and PRIKY 21199)the Fundamental Research Funds for the Central Universities(No.2462020BJRC008)the support of Energy Internet Research Center,China University of Petroleum(Beijing),Haihe Laboratory of Sustainable Chemical Transformations(No.CYZC202105)the Beijing Synchrotron Radiation Facility(BSRF)Shanghai Synchrotron Radiation Facility(SSRF)during the XAFS measurements at the beamline of 1W1B,1W2B,and BL11B.
文摘Methylcyclohexane(MCH)serves as an ideal hydrogen carrier in hydrogen storage and transportation process.In the continuous production of hydrogen from MCH dehydrogenation,the rational design of energy-efficient catalytic way with good performance remains an enormous challenge.Herein,an internal electric heating(IEH)assisted mode was designed and proposed by the directly electrical-driven catalyst using the resistive heating effect.The Pt/Al2O_(3)on Fe foam(Pt/Al2O_(3)/FF)with unique threedimensional network structure was constructed.The catalysts were studied in a comprehensive way including X-ray diffraction(XRD),scanning electron microscopy(SEM)-mapping,in situ extended X-ray absorption fine structure(EXAFS),and in situ COFourier transform infrared(FTIR)measurements.It was found that the hydrogen evolution rate in IEH mode can reach up to above 2060 mmol·gPt^(−1)·min^(−1),which is 2–5 times higher than that of reported Pt based catalysts under similar reaction conditions in conventional heating(CH)mode.In combination with measurements from high-resolution infrared thermometer,the equations of heat transfer rate,and reaction heat analysis results,the Pt/Al2O_(3)/FF not only has high mass and heat transfer ability to promote catalytic performance,but also behaves as the heating component with a low thermal resistance and heat capacity offering a fast temperature response in IEH mode.In addition,the chemical adsorption and activation of MCH molecules can be efficiently facilitated by IEH mode,proved by the operando MCH-FTIR results.Therefore,the as-developed IEH mode can efficiently reduce the heat and mass transfer limitations and prominently boost the dehydrogenation performance,which has a broad application potential in hydrogen storage and other catalytic reaction processes.