Spinel metal oxides containing Mn,Co,or Fe(AB_(2)O_(4),A/B=Mn/Fe/Co)are one of the most promising nonPt electrocatalysts for oxygen reduction reaction(ORR)in alkaline conditions.However,the low conductivity of metal o...Spinel metal oxides containing Mn,Co,or Fe(AB_(2)O_(4),A/B=Mn/Fe/Co)are one of the most promising nonPt electrocatalysts for oxygen reduction reaction(ORR)in alkaline conditions.However,the low conductivity of metal oxides and the poor intrinsic activities of transition metal sites lead to unsatisfactory ORR performance.In this study,eutectic molten salt(EMS)treatment is employed to reconstruct the atomic arrangement of MnFe_(2)O_(4)electrocatalyst as a prototype for enhancing ORR performance.Comprehensive analyses by using XAFS,soft XAS,XPS,and electrochemical methods reveal that the EMS treatment reduces the oxygen vacancies and spinel inverse in MnFe_(2)O_(4)effectively,which improves the electric conductivity and increases the population of more catalytically active Mn^(2+)sites with tetrahedral coordination.Moreover,the enhanced Mn-O interaction after EMS treatment is conducive to the adsorption and activation of O_(2),which promotes the first electron transfer step(generally considered as the ratedetermining step)of the ORR process.As a result,the EMS treated MnFe_(2)O_(4)catalyst delivers a positive shift of 40 mV in the ORR half-wave potential and a two-fold enhanced mass/specific activity.This work provides a convenient approach to manipulate the atomic architecture and local electronic structure of spinel oxides as ORR electrocatalysts and a comprehensive understanding of the structureperformance relationship from the molecular/atomic scale.展开更多
Efficient and convenient treatment of industrial dyeing wastewater is of great significance to guarantee human and animal health.This work presented the enhanced catalytic activity at pH 3.0 of laccase immobilized on ...Efficient and convenient treatment of industrial dyeing wastewater is of great significance to guarantee human and animal health.This work presented the enhanced catalytic activity at pH 3.0 of laccase immobilized on amino-functionalized ZnFe_(2)O_(4) nanoparticles(ZnFe_(2)O_(4)-laccase)and its application for the degradation of textile dyes.Due to the existence of a large number of oxygen vacancies on the surface of the ZnFe_(2)O_(4) nanoparticles,negative ions accumulated on the magnetic carriers,which resulted in a harsh optimal pH value of the ZnFe_(2)O_(4)-laccase.Laccase activity assays revealed that the ZnFe_(2)O_(4)-laccase possessed superior pH and thermal stabilities,excellent reusability,and noticeable organic solvent tolerance.Meanwhile,the ZnFe_(2)O_(4) laccase presented efficient and sustainable degradation of high concentrations of textile dyes.The initial decoloration efficiencies of malachite green(MG),brilliant green(BG),azophloxine,crystal violet(CV),reactive blue 19(RB19),and procion red MX-5B were approximately 99.1%,95.0%,93.3%,87.4%,86.1%,and 85.3%,respectively.After 10 consecutive reuses,the degradation rates of the textile dyes still maintained about 98.2%,92.5%,83.2%,81.5%,79.8%and 65.9%,respectively.The excellent dye degradation properties indicate that the ZnFe_(2)O_(4)-laccase has a technical application in high concentrations of dyestuff treatment.展开更多
The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrot...The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.展开更多
基金supported by the National Natural Science Foundation of China (12241502,52002367)the Fundamental Research Funds for the Central Universities (20720220010)the National Key Research and Development Program of China (2019YFA0405602)。
文摘Spinel metal oxides containing Mn,Co,or Fe(AB_(2)O_(4),A/B=Mn/Fe/Co)are one of the most promising nonPt electrocatalysts for oxygen reduction reaction(ORR)in alkaline conditions.However,the low conductivity of metal oxides and the poor intrinsic activities of transition metal sites lead to unsatisfactory ORR performance.In this study,eutectic molten salt(EMS)treatment is employed to reconstruct the atomic arrangement of MnFe_(2)O_(4)electrocatalyst as a prototype for enhancing ORR performance.Comprehensive analyses by using XAFS,soft XAS,XPS,and electrochemical methods reveal that the EMS treatment reduces the oxygen vacancies and spinel inverse in MnFe_(2)O_(4)effectively,which improves the electric conductivity and increases the population of more catalytically active Mn^(2+)sites with tetrahedral coordination.Moreover,the enhanced Mn-O interaction after EMS treatment is conducive to the adsorption and activation of O_(2),which promotes the first electron transfer step(generally considered as the ratedetermining step)of the ORR process.As a result,the EMS treated MnFe_(2)O_(4)catalyst delivers a positive shift of 40 mV in the ORR half-wave potential and a two-fold enhanced mass/specific activity.This work provides a convenient approach to manipulate the atomic architecture and local electronic structure of spinel oxides as ORR electrocatalysts and a comprehensive understanding of the structureperformance relationship from the molecular/atomic scale.
基金supported by the National Natural Science Foundation of China(21471002)Scientific Research Projects of Universities in Anhui Province(2022AH040135)+1 种基金Natural Science Research Project for Anhui Universities(KJ2021A0509)Anhui Natural Science Foundation(2208085MC83).
文摘Efficient and convenient treatment of industrial dyeing wastewater is of great significance to guarantee human and animal health.This work presented the enhanced catalytic activity at pH 3.0 of laccase immobilized on amino-functionalized ZnFe_(2)O_(4) nanoparticles(ZnFe_(2)O_(4)-laccase)and its application for the degradation of textile dyes.Due to the existence of a large number of oxygen vacancies on the surface of the ZnFe_(2)O_(4) nanoparticles,negative ions accumulated on the magnetic carriers,which resulted in a harsh optimal pH value of the ZnFe_(2)O_(4)-laccase.Laccase activity assays revealed that the ZnFe_(2)O_(4)-laccase possessed superior pH and thermal stabilities,excellent reusability,and noticeable organic solvent tolerance.Meanwhile,the ZnFe_(2)O_(4) laccase presented efficient and sustainable degradation of high concentrations of textile dyes.The initial decoloration efficiencies of malachite green(MG),brilliant green(BG),azophloxine,crystal violet(CV),reactive blue 19(RB19),and procion red MX-5B were approximately 99.1%,95.0%,93.3%,87.4%,86.1%,and 85.3%,respectively.After 10 consecutive reuses,the degradation rates of the textile dyes still maintained about 98.2%,92.5%,83.2%,81.5%,79.8%and 65.9%,respectively.The excellent dye degradation properties indicate that the ZnFe_(2)O_(4)-laccase has a technical application in high concentrations of dyestuff treatment.
基金This work was supported by the National Natural Science Foundation of China(No.51477002)the University Synergy Innovation Program of Anhui Province,China(No.GXXT-2019-028).
文摘The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.
