Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(...Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.展开更多
Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts wer...Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.展开更多
Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts...Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios x.The NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of reactants.The optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after K-poisoning.The interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox capability.However,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi catalyst.Finally,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on 10.SSFeCeVWTi catalyst.These results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.展开更多
Flexible multifunctional polymer-based electromagnetic interference(EMI)shielding composite films have important application values in the fields of 5G communication technology,wearable electronic devices and artifici...Flexible multifunctional polymer-based electromagnetic interference(EMI)shielding composite films have important application values in the fields of 5G communication technology,wearable electronic devices and artificial intelligence.In this work,Fe_(3)O_(4)/polyamic acid(PAA)nanofiber films are prepared by in-situ polymerization and electrospinning technology,and Ti_(3)C_(2)T_(x)nanosheets are deposited on the surface of the Fe_(3)O_(4)/PAA nanofiber films via vacuum-assisted filtration.Then,Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/polyimide(PI))composite films are obtained by thermal imidization.The two sides of the Janus films exhibit completely different properties.The Fe_(3)O_(4)/PI side has excellent hydrophobicity and insulation property,and the Ti_(3)C_(2)T_(x)side has hydrophilicity and terrific conductivity.When the mass fraction of Ti_(3)C_(2)T_(x)is 80 wt.%,the Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/PI)composite film has excellent EMI shielding performances and mechanical properties,with EMI shielding effectiveness,tensile strength and Young’s modulus reaching 66 dB,114.5 MPa and 5.8 GPa,respectively.At the same time,electromagnetic waves show different absorption shielding effectiveness(SEA)when incident from two sides of the Janus films.When the electromagnetic waves are incident from the Fe_(3)O_(4)/PI side,the SEA of the Janus film is 58 dB,much higher than that when the electromagnetic waves are incident from the Ti_(3)C_(2)T_(x)side(39 dB).In addition,the Ti_(3)C_(2)T_(x)side of the Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/PI)composite films also has excellent electrothermal and photothermal conversion performances.When the applied voltage is 4 V,the stable surface temperature reaches 108°C;when it is irradiated by simulated sunlight with power density of 200 mW/cm2,the stable surface temperature reaches 95℃.展开更多
Ethylene carbonate(EC)is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity,relatively stable solid electrolyte interphase(SEI),and wide electrochemical window.E...Ethylene carbonate(EC)is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity,relatively stable solid electrolyte interphase(SEI),and wide electrochemical window.EC is also the most widely used electrolyte solvent in sodium ion batteries.However,compared to lithium metal,sodium metal(Na)shows higher activity and reacts violently with EC-based electrolyte(NaPF_(6)as solute),which leads to the failure of sodium metal batteries(SMBs).Herein,we reveal the electrochemical instability mechanism of EC on sodium metal battery,and find that the com-bination of EC and NaPF_(6) is electrically reduced in sodium metal anode during charging,resulting in the reduction of the first coulombic efficiency,and the continuous consumption of electrolyte leads to the cell failure.To address the above issues,an additive modified linear carbonate-based electrolyte is provided as a substitute for EC based electrolytes.Specifically,ethyl methyl carbonate(EMC)and dimethyl carbon-ate(DMC)as solvents and fluoroethylene carbonate(FEC)as SEI-forming additive have been identified as the optimal solvent for NaFP_(6)based electrolyte and used in Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))/Na batteries.The batter-ies exhibit excellent capacity retention rate of about 80%over 1000 cycles at a cut-off voltage of 4.3 V.展开更多
在病毒感染和癌症治疗中,干扰素α-2b(IFN-α2b)的灵敏检测至关重要,因此需要开发经济、稳定的灵敏检测IFN-α2b的方法.传统的酶联免疫吸附测定(ELISA)中使用的天然酶存在制备成本高和稳定性差等问题.为了提高其灵敏度并降低成本,我们...在病毒感染和癌症治疗中,干扰素α-2b(IFN-α2b)的灵敏检测至关重要,因此需要开发经济、稳定的灵敏检测IFN-α2b的方法.传统的酶联免疫吸附测定(ELISA)中使用的天然酶存在制备成本高和稳定性差等问题.为了提高其灵敏度并降低成本,我们合成了聚乙烯亚胺(PEI)修饰的四氧化三铁磁性纳米粒子(Fe_(3)O_(4)@PEI MNPs).在基于ELISA的IFN-α2b检测中,这些磁性纳米粒子作为辣根过氧化物酶的替代品,提供了比色谱和传统ELISA技术更高的灵敏度,并且能够实现IFN-α2b的可视化检测.该免疫分析方法的线性范围为0.075-25 ng mL^(-1),检测限为0.055 ng mL^(-1).基于Fe_(3)O_(4)@PEI MNPs优异的过氧化物酶活性,该方法在用于检测IFN-α2b和其他蛋白质生物标志物监测方面具有临床应用潜力.展开更多
基金support from the National Natural Science Foundation of China(51402100,21905088,21573066 and U19A2017)the Provincial Natural Science Foundation of Hunan(2020JJ5044,2022JJ10006)。
文摘Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous challenges.Herein,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)activity.In view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and Ni.The optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron spectroscopy.With the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.
文摘Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.
基金Project supported by Fujian Provincial Department of Science and Technology,China (2020Y0085)Youth Innovation Promotion Association,Chinese Academy of Sciences (2020309)the Cultivating Project of Strategic Priority Research Program of Chinese Academy of Sciences (XDPB1902)。
文摘Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios x.The NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of reactants.The optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after K-poisoning.The interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox capability.However,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi catalyst.Finally,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on 10.SSFeCeVWTi catalyst.These results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.
基金supports from the National Natural Science Foundation of China(Nos.U21A2093 and 51903145)Fundamental Research Funds for the Central Universities(No.D5000210627)+1 种基金Y.L.Z.would like to thank the Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University(No.CX2021107)This work is also financially supported by Polymer Electromagnetic Functional Materials Innovation Team of Shaanxi Sanqin Scholars.
文摘Flexible multifunctional polymer-based electromagnetic interference(EMI)shielding composite films have important application values in the fields of 5G communication technology,wearable electronic devices and artificial intelligence.In this work,Fe_(3)O_(4)/polyamic acid(PAA)nanofiber films are prepared by in-situ polymerization and electrospinning technology,and Ti_(3)C_(2)T_(x)nanosheets are deposited on the surface of the Fe_(3)O_(4)/PAA nanofiber films via vacuum-assisted filtration.Then,Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/polyimide(PI))composite films are obtained by thermal imidization.The two sides of the Janus films exhibit completely different properties.The Fe_(3)O_(4)/PI side has excellent hydrophobicity and insulation property,and the Ti_(3)C_(2)T_(x)side has hydrophilicity and terrific conductivity.When the mass fraction of Ti_(3)C_(2)T_(x)is 80 wt.%,the Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/PI)composite film has excellent EMI shielding performances and mechanical properties,with EMI shielding effectiveness,tensile strength and Young’s modulus reaching 66 dB,114.5 MPa and 5.8 GPa,respectively.At the same time,electromagnetic waves show different absorption shielding effectiveness(SEA)when incident from two sides of the Janus films.When the electromagnetic waves are incident from the Fe_(3)O_(4)/PI side,the SEA of the Janus film is 58 dB,much higher than that when the electromagnetic waves are incident from the Ti_(3)C_(2)T_(x)side(39 dB).In addition,the Ti_(3)C_(2)T_(x)side of the Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/PI)composite films also has excellent electrothermal and photothermal conversion performances.When the applied voltage is 4 V,the stable surface temperature reaches 108°C;when it is irradiated by simulated sunlight with power density of 200 mW/cm2,the stable surface temperature reaches 95℃.
基金supported by the National Natural Science Foundation of China(52172201,51732005,51902118,and 52102249)the China Postdoctoral Science Foundation(2019M662609and 2020T130217)for financial support。
文摘Ethylene carbonate(EC)is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity,relatively stable solid electrolyte interphase(SEI),and wide electrochemical window.EC is also the most widely used electrolyte solvent in sodium ion batteries.However,compared to lithium metal,sodium metal(Na)shows higher activity and reacts violently with EC-based electrolyte(NaPF_(6)as solute),which leads to the failure of sodium metal batteries(SMBs).Herein,we reveal the electrochemical instability mechanism of EC on sodium metal battery,and find that the com-bination of EC and NaPF_(6) is electrically reduced in sodium metal anode during charging,resulting in the reduction of the first coulombic efficiency,and the continuous consumption of electrolyte leads to the cell failure.To address the above issues,an additive modified linear carbonate-based electrolyte is provided as a substitute for EC based electrolytes.Specifically,ethyl methyl carbonate(EMC)and dimethyl carbon-ate(DMC)as solvents and fluoroethylene carbonate(FEC)as SEI-forming additive have been identified as the optimal solvent for NaFP_(6)based electrolyte and used in Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7))/Na batteries.The batter-ies exhibit excellent capacity retention rate of about 80%over 1000 cycles at a cut-off voltage of 4.3 V.
基金financially supported by the National Key Research and Development Program of China(2019YFA0709202)the Natural Science Foundation of Jilin Province(20220101055JC)+1 种基金the International Cooperation Project of Jilin Scientific and Technological Development Program(20190701059GH)the Department of Science and Technology of Jilin Province(20220508098RC)。
文摘在病毒感染和癌症治疗中,干扰素α-2b(IFN-α2b)的灵敏检测至关重要,因此需要开发经济、稳定的灵敏检测IFN-α2b的方法.传统的酶联免疫吸附测定(ELISA)中使用的天然酶存在制备成本高和稳定性差等问题.为了提高其灵敏度并降低成本,我们合成了聚乙烯亚胺(PEI)修饰的四氧化三铁磁性纳米粒子(Fe_(3)O_(4)@PEI MNPs).在基于ELISA的IFN-α2b检测中,这些磁性纳米粒子作为辣根过氧化物酶的替代品,提供了比色谱和传统ELISA技术更高的灵敏度,并且能够实现IFN-α2b的可视化检测.该免疫分析方法的线性范围为0.075-25 ng mL^(-1),检测限为0.055 ng mL^(-1).基于Fe_(3)O_(4)@PEI MNPs优异的过氧化物酶活性,该方法在用于检测IFN-α2b和其他蛋白质生物标志物监测方面具有临床应用潜力.
