La2Zr2O7 thermal barrier coatings(TBCs) with dispersed Pt particles were prepared by cathode plasma electrolytic deposition(CPED) with ceramic balls added to the cathode region. Compared with the conventional CPED...La2Zr2O7 thermal barrier coatings(TBCs) with dispersed Pt particles were prepared by cathode plasma electrolytic deposition(CPED) with ceramic balls added to the cathode region. Compared with the conventional CPED, when ceramic balls are used in the cathode region, the plasma discharge ignition current density decreases approximately 62-fold and the stable plasma discharges occur at the whole cathode surface. Such TBCs with a thickness of 100 μm exhibit a crack-free surface and are composed of pyrochlore-structured La2Zr2O7. Cyclic oxidation, scratching, and thermal insulation capability tests show that such TBCs not only exhibit high resistance to oxidation and spallation but also provide good thermal insulation. These beneficial effects are attributed to the excellent properties of TBCs, such as good thermal insulation because of low thermal conductivity, high-temperature oxidation resistance because of low-oxygen diffusion rate, and good mechanical properties because of the toughening effect of Pt particles.展开更多
New composition perovskite-type compounds with formula Sr0.6Bi0.4FeO2.7,Sr1-xBixFeO3-y(x=0.1 to 0. 9 in interveral of 0.1),and Ba1.5Pt0.5Mn2O6 have been synthsized and structurally characterized.The crystal structure ...New composition perovskite-type compounds with formula Sr0.6Bi0.4FeO2.7,Sr1-xBixFeO3-y(x=0.1 to 0. 9 in interveral of 0.1),and Ba1.5Pt0.5Mn2O6 have been synthsized and structurally characterized.The crystal structure of Sr0.6Bi0.4FeO2.7has been determined by X-ray single crystal diffraction,and the data of neutron powder diffraction collected at both room temperature and elevated temperature(380℃).The compound Sr0.6Bi0.4FeO2.7 crystallizes in the cubic space group of Pm3m with Z=1,a=3.9330(6) at room temperature,a=3.9498(6)A at 380℃.The magnetic structure from the neutron powder diffraction data collected at room temperature is consistent with a simple G-type antiferromagnetism and has a magnetic moment of 4.98 μB per Fe atom.The structures of Sr1-xBixFeO3-y with x other than 0.4 were also refined from the X-ray powder diffraction data.The data were consistent with a tetragonal cell when x=0.1,a rhombohedral cell when x= 0.9,and a cubic cell for x=0.2~0.8.From single crystal X-ray diffraction data,Ba1.5Pt0.5Mn2O6 crystallizes in hexagonal space group of P63mc with a= 5.7722 (6),c=4.4504(9),V=128.42(2),Z=1.The Sr(1-x)BixFeO(3-y)are found to be a good electronic and ionic conductor.展开更多
A microelectrode glucose biosensor based on a three-dimensional hybrid nanoporous platinum/graphene oxide nanostructure was developed for rapid glucose detection of tomato and cucumber fruits.The nanostructure was fab...A microelectrode glucose biosensor based on a three-dimensional hybrid nanoporous platinum/graphene oxide nanostructure was developed for rapid glucose detection of tomato and cucumber fruits.The nanostructure was fabricated by a two-step modification method on a microelectrode for loading a larger amount of glucose oxidase.The nanoporous structure was prepared on the surface of the platinum microelectrode by electrochemical etching,and then graphene oxide was deposited on the prepared nanoporous electrode by electrochemical deposition.The nanoporous platinum/graphene oxide nanostructure had the advantage of improving the effective surface area of the electrode and the loading quantity of glucose oxidase.As a result,the biosensor achieved a wide range of 0.1-20.0 mmol/L in glucose detection,which had the ability to accurately detect the glucose content.It was found that the three-dimensional hybrid nanostructure on the electrode surface realized the rapid direct electrochemistry of glucose oxidase.Therefore,the biosensor achieved high glucose detection sensitivity 11.64μA·L/(mmol.cm^(2)),low detection limit(13μmol/L)and rapid response time(reaching 95%steady-state response within 3 s),when calibrating in glucose standard solution.In agricultural application,the as-prepared biosensor was employed to detect the glucose concentration of tomato and cucumber samples.The results showed that the relative deviation of this method was less than 5%when compared with that of high-performance liquid chromatography,implying high accuracy of the presented biosensor in glucose detection in plants.展开更多
Synthesis of shape-controlled Pt nanocrystals is substantial and important for enhancing chemical and electrochemical reactions.However,the removal of capping agents,shape-controlling chemicals,on Pt surfaces is essen...Synthesis of shape-controlled Pt nanocrystals is substantial and important for enhancing chemical and electrochemical reactions.However,the removal of capping agents,shape-controlling chemicals,on Pt surfaces is essential prior to conducting the catalytic reactions.Here we report a facile one-pot synthesis of Pt nanocubes directly grown on carbon supports(Pt nanocubes/C) with modulating the kinetic reaction factors for shaping the nanocrystals,but without adding any capping agents for preserving the clean Pt surfaces.Well-dispersed Pt nanocubes/C shows enhanced activity and long-term stability toward methanol oxidation reaction compared to the commercial Pt/C catalyst.展开更多
Surfactant removal from the surface of platinum-based nanoparticles prepared using solution-based methods is a prerequisite to realize their high catalytic performance for electrochemical reactions. Herein, we report ...Surfactant removal from the surface of platinum-based nanoparticles prepared using solution-based methods is a prerequisite to realize their high catalytic performance for electrochemical reactions. Herein, we report an effective approach combining acetic acid refluxing with an electrochemical process for the removal of amine- or thiol-based capping agents from the surface of supported-platinum nanoparticles. This strategy involves surfactant protonation by refluxing the supported-platinum particles in acetic acid followed by surfactant removal by subsequent electrochemical treatment at high potential. We demon- strate that this combined activation process is essential to enhance platinum particle performance in catalyzing direct methanol fuel cell reactions, including methanol oxidation and oxygen reduction reac- tions. The studies in this work show promise in electrocatalysis applications of solution-based materials synthesis.展开更多
Understanding how defect chemistry of oxide material influences the thermal stability of noble metal dopant ions plays an important role in designing high-performance heterogeneous catalytic systems.Here we use in-sit...Understanding how defect chemistry of oxide material influences the thermal stability of noble metal dopant ions plays an important role in designing high-performance heterogeneous catalytic systems.Here we use in-situ ambient-pressure X-ray photoemission spectroscopy(APXPS)to experimentally determine the role of grain boundary in the thermal stability of platinum doped cerium oxide(Pt/CeO_(2)).The grain boundaries were introduced in Pt/CeO_(2)thin films by pulsed laser deposition without significantly change of the surface microstructure.The defect level was tuned by the strain field obtained using a highly/low mismatched substrate.The Pt/CeO_(2)thin film models having well defined crystallographic properties but different grain boundary structural defect levels provide an ideal platform for exploring the evolution of Pt–O–Ce bond with changing the temperature in reducing conditions.We have direct demonstration and explanation of the role of Ce^(3+)induced by grain boundaries in enhancing Pt2+stability.We observe that the Pt^(2+)–O–Ce^(3+)bond provides an ideal coordinated site for anchoring of Pt^(2+)ions and limits the further formation of oxygen vacancies during the reduction with H_(2).Our findings demonstrate the importance of grain boundary in the atomic-scale design of thermally stable catalytic active sites.展开更多
PtSnNa/γ-Al2O3 catalyst is widely used in the dehydrogenation of light alkane. This paper reports a new fabrication method of the catalyst. In the work, γ-Al2O3, SnCl4 and NaCl were ball milled to upload Sn and Na+...PtSnNa/γ-Al2O3 catalyst is widely used in the dehydrogenation of light alkane. This paper reports a new fabrication method of the catalyst. In the work, γ-Al2O3, SnCl4 and NaCl were ball milled to upload Sn and Na+ onto the support instead of the conventionally used immersion method. The subsequent baking procedures frimly fixed Sn onto the support, which could disperse Pt introduced by immersion. The effects of Sn and Na+ additives on the catalytic performance of PtSnNa/y-Al2O3 catalyst were investigated. It was found that the appropriate molar ratio of Sn/Pt was 6:1 while the favorable weight percentage of Na+ was 0.90%. Compared with the reaction catalyzed by the industrially employed PtSnNa/ γ-Al2O3 catalyst, the conversion of propane and the selectivity of propylene had been greatly improved, which were 26.97%; and 99.18% respectivelv after 12 h reaction.展开更多
基金financially supported by the National Natural Science Foundation of China (No. 51271030)
文摘La2Zr2O7 thermal barrier coatings(TBCs) with dispersed Pt particles were prepared by cathode plasma electrolytic deposition(CPED) with ceramic balls added to the cathode region. Compared with the conventional CPED, when ceramic balls are used in the cathode region, the plasma discharge ignition current density decreases approximately 62-fold and the stable plasma discharges occur at the whole cathode surface. Such TBCs with a thickness of 100 μm exhibit a crack-free surface and are composed of pyrochlore-structured La2Zr2O7. Cyclic oxidation, scratching, and thermal insulation capability tests show that such TBCs not only exhibit high resistance to oxidation and spallation but also provide good thermal insulation. These beneficial effects are attributed to the excellent properties of TBCs, such as good thermal insulation because of low thermal conductivity, high-temperature oxidation resistance because of low-oxygen diffusion rate, and good mechanical properties because of the toughening effect of Pt particles.
文摘New composition perovskite-type compounds with formula Sr0.6Bi0.4FeO2.7,Sr1-xBixFeO3-y(x=0.1 to 0. 9 in interveral of 0.1),and Ba1.5Pt0.5Mn2O6 have been synthsized and structurally characterized.The crystal structure of Sr0.6Bi0.4FeO2.7has been determined by X-ray single crystal diffraction,and the data of neutron powder diffraction collected at both room temperature and elevated temperature(380℃).The compound Sr0.6Bi0.4FeO2.7 crystallizes in the cubic space group of Pm3m with Z=1,a=3.9330(6) at room temperature,a=3.9498(6)A at 380℃.The magnetic structure from the neutron powder diffraction data collected at room temperature is consistent with a simple G-type antiferromagnetism and has a magnetic moment of 4.98 μB per Fe atom.The structures of Sr1-xBixFeO3-y with x other than 0.4 were also refined from the X-ray powder diffraction data.The data were consistent with a tetragonal cell when x=0.1,a rhombohedral cell when x= 0.9,and a cubic cell for x=0.2~0.8.From single crystal X-ray diffraction data,Ba1.5Pt0.5Mn2O6 crystallizes in hexagonal space group of P63mc with a= 5.7722 (6),c=4.4504(9),V=128.42(2),Z=1.The Sr(1-x)BixFeO(3-y)are found to be a good electronic and ionic conductor.
基金funded by the Key-Area Research and Development Program of Guangdong Province (2019B020219002)the Characteristic Innovation Project of Ordinary University of Guangdong Province (2019KTSCX018)+1 种基金the Guangdong Natural Science Funds for Distinguished Young Scholar (2014A030306005)the Guangdong Basic and Applied Basic Research Foundation (2019A1515110929),China.
文摘A microelectrode glucose biosensor based on a three-dimensional hybrid nanoporous platinum/graphene oxide nanostructure was developed for rapid glucose detection of tomato and cucumber fruits.The nanostructure was fabricated by a two-step modification method on a microelectrode for loading a larger amount of glucose oxidase.The nanoporous structure was prepared on the surface of the platinum microelectrode by electrochemical etching,and then graphene oxide was deposited on the prepared nanoporous electrode by electrochemical deposition.The nanoporous platinum/graphene oxide nanostructure had the advantage of improving the effective surface area of the electrode and the loading quantity of glucose oxidase.As a result,the biosensor achieved a wide range of 0.1-20.0 mmol/L in glucose detection,which had the ability to accurately detect the glucose content.It was found that the three-dimensional hybrid nanostructure on the electrode surface realized the rapid direct electrochemistry of glucose oxidase.Therefore,the biosensor achieved high glucose detection sensitivity 11.64μA·L/(mmol.cm^(2)),low detection limit(13μmol/L)and rapid response time(reaching 95%steady-state response within 3 s),when calibrating in glucose standard solution.In agricultural application,the as-prepared biosensor was employed to detect the glucose concentration of tomato and cucumber samples.The results showed that the relative deviation of this method was less than 5%when compared with that of high-performance liquid chromatography,implying high accuracy of the presented biosensor in glucose detection in plants.
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF) funded by the Ministry of Education(NRF-2015R1D1A3A01019467,NRF2017R1D1A1B03031892) and KBSI(D37614)
文摘Synthesis of shape-controlled Pt nanocrystals is substantial and important for enhancing chemical and electrochemical reactions.However,the removal of capping agents,shape-controlling chemicals,on Pt surfaces is essential prior to conducting the catalytic reactions.Here we report a facile one-pot synthesis of Pt nanocubes directly grown on carbon supports(Pt nanocubes/C) with modulating the kinetic reaction factors for shaping the nanocrystals,but without adding any capping agents for preserving the clean Pt surfaces.Well-dispersed Pt nanocubes/C shows enhanced activity and long-term stability toward methanol oxidation reaction compared to the commercial Pt/C catalyst.
文摘Surfactant removal from the surface of platinum-based nanoparticles prepared using solution-based methods is a prerequisite to realize their high catalytic performance for electrochemical reactions. Herein, we report an effective approach combining acetic acid refluxing with an electrochemical process for the removal of amine- or thiol-based capping agents from the surface of supported-platinum nanoparticles. This strategy involves surfactant protonation by refluxing the supported-platinum particles in acetic acid followed by surfactant removal by subsequent electrochemical treatment at high potential. We demon- strate that this combined activation process is essential to enhance platinum particle performance in catalyzing direct methanol fuel cell reactions, including methanol oxidation and oxygen reduction reac- tions. The studies in this work show promise in electrocatalysis applications of solution-based materials synthesis.
基金The APXPS experiments were performed at BL02B01 of SSRF with the approval of the Proposal Assessing Committee of SiP.ME2 platform project(Proposal No.2019-SSRF-PT-011613)the Natural Science Foundation of China(No.11227902)the Shanghai Key Research Program(No.20ZR1436700).
文摘Understanding how defect chemistry of oxide material influences the thermal stability of noble metal dopant ions plays an important role in designing high-performance heterogeneous catalytic systems.Here we use in-situ ambient-pressure X-ray photoemission spectroscopy(APXPS)to experimentally determine the role of grain boundary in the thermal stability of platinum doped cerium oxide(Pt/CeO_(2)).The grain boundaries were introduced in Pt/CeO_(2)thin films by pulsed laser deposition without significantly change of the surface microstructure.The defect level was tuned by the strain field obtained using a highly/low mismatched substrate.The Pt/CeO_(2)thin film models having well defined crystallographic properties but different grain boundary structural defect levels provide an ideal platform for exploring the evolution of Pt–O–Ce bond with changing the temperature in reducing conditions.We have direct demonstration and explanation of the role of Ce^(3+)induced by grain boundaries in enhancing Pt2+stability.We observe that the Pt^(2+)–O–Ce^(3+)bond provides an ideal coordinated site for anchoring of Pt^(2+)ions and limits the further formation of oxygen vacancies during the reduction with H_(2).Our findings demonstrate the importance of grain boundary in the atomic-scale design of thermally stable catalytic active sites.
基金the Doctoral Program of Higher Education(No. SRFDP-2012009111001)NNSFC(No. 21202141)+1 种基金Priority Academic Program Development(PAPD) of Jiangsu Higher Education Institutions, Key Science & Technology Specific Projects of Yangzhou(No. YZ20122029)Yangzhou Nature Science Foundation(No. YZ2014040) for financial support
文摘PtSnNa/γ-Al2O3 catalyst is widely used in the dehydrogenation of light alkane. This paper reports a new fabrication method of the catalyst. In the work, γ-Al2O3, SnCl4 and NaCl were ball milled to upload Sn and Na+ onto the support instead of the conventionally used immersion method. The subsequent baking procedures frimly fixed Sn onto the support, which could disperse Pt introduced by immersion. The effects of Sn and Na+ additives on the catalytic performance of PtSnNa/y-Al2O3 catalyst were investigated. It was found that the appropriate molar ratio of Sn/Pt was 6:1 while the favorable weight percentage of Na+ was 0.90%. Compared with the reaction catalyzed by the industrially employed PtSnNa/ γ-Al2O3 catalyst, the conversion of propane and the selectivity of propylene had been greatly improved, which were 26.97%; and 99.18% respectivelv after 12 h reaction.