The phase evolution in (88%-91%)Mg-8%Sn-l%Zn-X (X=A1, Mn and/or Ce) system was analyzed via CALPHAD method and simulations were used in precise selection of the chemical composition. The influence of the addition ...The phase evolution in (88%-91%)Mg-8%Sn-l%Zn-X (X=A1, Mn and/or Ce) system was analyzed via CALPHAD method and simulations were used in precise selection of the chemical composition. The influence of the addition of different alloying elements such as A1, Mn and Ce on the microstructure and microhardness of Mg-8%Sn-l%Zn-based alloys was investigated. Combined addition of A1 and Mn shows features distinct from separate addition of A1 or Mn. Additions of l%AI and l%Mn to base alloy result in the formation of massive A1-Mn phase in a-Mg matrix grains. Addition of Ce element can refme the second eutectic precipitates and form intermetallic compounds with Sn. Fine rod-like Sn-Ce phase presents mainly on the grain boundaries and plays a role in inhibiting grain growth. The effects of alloying elements on Vickers microhardness and indentation size effect of base alloy were examined.展开更多
Fischer-Tropsch synthesis (FTS) is an increasingly important approach for producing liquid fuels and chemicals via syngas-that is, synthesis gas, a mixture of carbon monoxide and hydrogen-generated from coal, natura...Fischer-Tropsch synthesis (FTS) is an increasingly important approach for producing liquid fuels and chemicals via syngas-that is, synthesis gas, a mixture of carbon monoxide and hydrogen-generated from coal, natural gas, or biomass. In FTS, dispersed transition metal nanoparticles are used to catalyze the reactions underlying the formation of carbon-carbon bonds. Catalytic activity and selectivity are strongly correlated with the electronic and geometric structure of the nanoparticles, which depend on the particle size, morphology, and crystallographic phase of the nanoparticles. In this article, we review recent works dealing with the aspects of bulk and surface sensitivity of the FTS reaction. Understanding the different catalytic behavior in more detail as a function of these parameters may guide the design of more active, selective, and stable FTS catalysts.展开更多
Due to the oxygen storage and release properties,cerium zirconium mixed oxides are recognized as the key material in automotive three-way catalysts.To reveal the effects of co-precipitation temperature on structure,ph...Due to the oxygen storage and release properties,cerium zirconium mixed oxides are recognized as the key material in automotive three-way catalysts.To reveal the effects of co-precipitation temperature on structure,physical and chemical properties of multi-doped cerium zirconium mixed oxides,a series of La and Y doped cerium zirconium mixed oxides(CZLYs)were synthesized via a co-precipitation method,and the physical and chemical properties of CZLYs were systemically characterized by XRD,N_(2) adsorption−desorption,TEM,XPS,oxygen storage capacity(OSC)and hydrogen temperature programmed reduction(H_(2)-TPR).The results show that co-precipitation temperature is an important parameter to influence the crystal size,oxygen storage capacity and thermal stability of CZLYs.When the co-precipitation temperature was 60℃,the best redox properties and thermal stability of CZLYs were obtained.After thermal treatment at 1100℃for 10 h,the specific surface area and oxygen storage capacity of the corresponding aged sample were 15.42 m^(2)/g and 497.7μmol/g,respectively.In addition,a mechanism was proposed to reveal the effects of co-precipitation temperature on the structure and properties of CZLYs.展开更多
The dependence of starting materials and their initial grain sizes on the formation of gases (H2, CH4, C2H6 and C3Hs) during serpentinization was investigated by conducting hydrothermal experiments at 311℃ and 3 kb...The dependence of starting materials and their initial grain sizes on the formation of gases (H2, CH4, C2H6 and C3Hs) during serpentinization was investigated by conducting hydrothermal experiments at 311℃ and 3 kbar on olivine and peridotite with initial grain sizes ranging from 〈30 to 177 μm. Hydrocarbons (CH4, C2H6 and C3H8) were produced from reaction between dissolved CO2 in the starting fluids and HE formed during serpentinization, which were analyzed by Gas Chromatography. It was found that olivine serpentinization produced much less H2 and CH4 compared with those after peridotite alteration, while their C2H6 and C3H8 were identical. For example, for olivine with initial grain sizes of 〈30 μm, the amounts of HE and CH4 were 79.6 mmol/kg and 460 μmol/kg after 27 days, respectively. By contrast, the quantities of H2 and CH4 produced in experiment on peridotite with the same run duration were much larger, 119 mmol/kg and 1300 μmol/kg, respectively. This indicates that spinel and pyroxene in peridotite may increase the amounts of HE and hydrocarbons, possibly due to the catalytic effect of aluminum released by spinel and pyroxene during serpentinization. Moreover, the production of H2 and hydrocarbons is negatively correlated with initial grain sizes of the starting material, with smaller amounts of HE and hydrocarbons for larger initial grain sizes, indicating that the kinetics of serpentinization influences the formation of HE and hydrocarbons, possibly because of the lack of catalytic minerals for the starting material with larger grain sizes. This study suggests that olivine cannot completely represent peridotite during serpentinization, and that H2 and hydrocarbons in hydrothermal fields near the mid-ocean ridge may be produced in a very long period of serpentinization or the presence of catalytic minerals due to large grain sizes of ultramafic rocks.展开更多
Two-dimensional(2D)transition metal chalcogenides(TMCs)are promising for nanoelectronics and energy applications.Among them,the emerging non-layered TMCs are unique due to their unsaturated dangling bonds on the surfa...Two-dimensional(2D)transition metal chalcogenides(TMCs)are promising for nanoelectronics and energy applications.Among them,the emerging non-layered TMCs are unique due to their unsaturated dangling bonds on the surface and strong intralayer and interlayer bonding.However,the synthesis of non-layered 2D TMCs is challenging and this has made it difficult to study their structures and properties at thin thickness limit.Here,we develop a universal dual-metal precursors method to grow non-layered TMCs in which a mixture of a metal and its chloride serves as the metal source.Taking hexagonal Fe_(1-x)S as an example,the thickness of the Fe_(1-x)S flakes is down to 3 nm with a lateral size of over 100 μm.Importantly,we find ordered cation Fe vacancies in Fe_(1-x)S,which is distinct from layered TMCs like MoS_(2) where anion vacancies are commonly observed.Low-temperature transport measurements and theoretical calculations show that 2D Fe_(1-x)S is a stable semiconductor with a narrow bandgap of60 meV.In addition to Fe_(1-x)S,the method is universal in growing various non-layered 2D TMCs containing ordered cation vacancies,including Fe_(1-x)Se,Co_(1-x)S,Cr_(1-x)S,and V_(1-x)S.This work paves the way to grow and exploit properties of non-layered materials at 2D thickness limit.展开更多
As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds...As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds(boehmite and alumina) on SOA yield and aerosol size in m-xylene/NOx photo-oxidation were investigated in a 2 m3 smog chamber at 30°C and 50% relative humidity. Compared to the seed-free system, the presence of aluminium seeds resulted in an increase in the SOA yield, and also enhanced the O3 concentration in the chamber. The photolysis of O3 is a major source of OH radical, which is the most important oxidant of m-xylene. The increase in O3 concentration could result in the generation of more OH radicals, and finally contribute to the SOA formation. Seed particles influence the SOA size mainly by acting as condensation nuclei. Semi-volatile organic compounds(SVOCs) were condensed onto these nuclei, resulting in the increase in SOA size. However, when aluminium seeds with high concentrations were introduced into the system, SVOCs that had been condensed onto each particle were dispersed by these seeds, leading to the reduction in aerosol size.展开更多
The thermodynamic properties of a binary self-condensing vinyl polymerization system consisting of monomers and inimers are investigated by the principle of statistical mechanics.In detail,in terms of two types of can...The thermodynamic properties of a binary self-condensing vinyl polymerization system consisting of monomers and inimers are investigated by the principle of statistical mechanics.In detail,in terms of two types of canonical partition functions constructed from different viewpoints,the equilibrium free energy,the law of mass action and the size distribution of hyperbranched polymers are obtained.As an application,the specific heat,equation of state and isothermal compressibility concerning the polymerization are given as well.To study the dimension of hyperbranched polymers in the system,a recursion formula satisfied by the(k+1)-th and k-th mean square radius of gyration is derived,and then the first,second and third radius of gyration under different solvent conditions are presented.The influences of the fraction of inimers,the conversion of vinyl groups and the solvent effect on the average dimension of hyperbranched polymers are discussed.展开更多
文摘The phase evolution in (88%-91%)Mg-8%Sn-l%Zn-X (X=A1, Mn and/or Ce) system was analyzed via CALPHAD method and simulations were used in precise selection of the chemical composition. The influence of the addition of different alloying elements such as A1, Mn and Ce on the microstructure and microhardness of Mg-8%Sn-l%Zn-based alloys was investigated. Combined addition of A1 and Mn shows features distinct from separate addition of A1 or Mn. Additions of l%AI and l%Mn to base alloy result in the formation of massive A1-Mn phase in a-Mg matrix grains. Addition of Ce element can refme the second eutectic precipitates and form intermetallic compounds with Sn. Fine rod-like Sn-Ce phase presents mainly on the grain boundaries and plays a role in inhibiting grain growth. The effects of alloying elements on Vickers microhardness and indentation size effect of base alloy were examined.
基金financial support by NWO-VICI and NWO-TOP grants awarded to Emiel J.M.Hensen
文摘Fischer-Tropsch synthesis (FTS) is an increasingly important approach for producing liquid fuels and chemicals via syngas-that is, synthesis gas, a mixture of carbon monoxide and hydrogen-generated from coal, natural gas, or biomass. In FTS, dispersed transition metal nanoparticles are used to catalyze the reactions underlying the formation of carbon-carbon bonds. Catalytic activity and selectivity are strongly correlated with the electronic and geometric structure of the nanoparticles, which depend on the particle size, morphology, and crystallographic phase of the nanoparticles. In this article, we review recent works dealing with the aspects of bulk and surface sensitivity of the FTS reaction. Understanding the different catalytic behavior in more detail as a function of these parameters may guide the design of more active, selective, and stable FTS catalysts.
基金the Hebei Key Research and Development Program,China(No.20374202D)the Hebei High Level Talent Team Building,China(No.205A1104H).
文摘Due to the oxygen storage and release properties,cerium zirconium mixed oxides are recognized as the key material in automotive three-way catalysts.To reveal the effects of co-precipitation temperature on structure,physical and chemical properties of multi-doped cerium zirconium mixed oxides,a series of La and Y doped cerium zirconium mixed oxides(CZLYs)were synthesized via a co-precipitation method,and the physical and chemical properties of CZLYs were systemically characterized by XRD,N_(2) adsorption−desorption,TEM,XPS,oxygen storage capacity(OSC)and hydrogen temperature programmed reduction(H_(2)-TPR).The results show that co-precipitation temperature is an important parameter to influence the crystal size,oxygen storage capacity and thermal stability of CZLYs.When the co-precipitation temperature was 60℃,the best redox properties and thermal stability of CZLYs were obtained.After thermal treatment at 1100℃for 10 h,the specific surface area and oxygen storage capacity of the corresponding aged sample were 15.42 m^(2)/g and 497.7μmol/g,respectively.In addition,a mechanism was proposed to reveal the effects of co-precipitation temperature on the structure and properties of CZLYs.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.4109037341121002+2 种基金41103012 and 41173069)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB06030100)also by Postdoctoral Science Foundation of China(Grant No.2015M570735)
文摘The dependence of starting materials and their initial grain sizes on the formation of gases (H2, CH4, C2H6 and C3Hs) during serpentinization was investigated by conducting hydrothermal experiments at 311℃ and 3 kbar on olivine and peridotite with initial grain sizes ranging from 〈30 to 177 μm. Hydrocarbons (CH4, C2H6 and C3H8) were produced from reaction between dissolved CO2 in the starting fluids and HE formed during serpentinization, which were analyzed by Gas Chromatography. It was found that olivine serpentinization produced much less H2 and CH4 compared with those after peridotite alteration, while their C2H6 and C3H8 were identical. For example, for olivine with initial grain sizes of 〈30 μm, the amounts of HE and CH4 were 79.6 mmol/kg and 460 μmol/kg after 27 days, respectively. By contrast, the quantities of H2 and CH4 produced in experiment on peridotite with the same run duration were much larger, 119 mmol/kg and 1300 μmol/kg, respectively. This indicates that spinel and pyroxene in peridotite may increase the amounts of HE and hydrocarbons, possibly due to the catalytic effect of aluminum released by spinel and pyroxene during serpentinization. Moreover, the production of H2 and hydrocarbons is negatively correlated with initial grain sizes of the starting material, with smaller amounts of HE and hydrocarbons for larger initial grain sizes, indicating that the kinetics of serpentinization influences the formation of HE and hydrocarbons, possibly because of the lack of catalytic minerals for the starting material with larger grain sizes. This study suggests that olivine cannot completely represent peridotite during serpentinization, and that H2 and hydrocarbons in hydrothermal fields near the mid-ocean ridge may be produced in a very long period of serpentinization or the presence of catalytic minerals due to large grain sizes of ultramafic rocks.
基金supported by the National Science Fund for Distinguished Young Scholars(52125309)the National Natural Science Foundation of China(51991343,51920105002,51991340,52188101,and 11974156)+3 种基金Guangdong Innovative and Entrepreneurial Research Team Program(2017ZT07C341 and 2019ZT08C044)the Bureau of Industry and Information Technology of Shenzhen for the “2017 Graphene Manufacturing Innovation Center Project”(201901171523)Shenzhen Basic Research Project(JCYJ20200109144616617 and JCYJ20190809180605522)Shenzhen Science and Technology Program(KQTD20190929173815000 and 20200925161102001)。
文摘Two-dimensional(2D)transition metal chalcogenides(TMCs)are promising for nanoelectronics and energy applications.Among them,the emerging non-layered TMCs are unique due to their unsaturated dangling bonds on the surface and strong intralayer and interlayer bonding.However,the synthesis of non-layered 2D TMCs is challenging and this has made it difficult to study their structures and properties at thin thickness limit.Here,we develop a universal dual-metal precursors method to grow non-layered TMCs in which a mixture of a metal and its chloride serves as the metal source.Taking hexagonal Fe_(1-x)S as an example,the thickness of the Fe_(1-x)S flakes is down to 3 nm with a lateral size of over 100 μm.Importantly,we find ordered cation Fe vacancies in Fe_(1-x)S,which is distinct from layered TMCs like MoS_(2) where anion vacancies are commonly observed.Low-temperature transport measurements and theoretical calculations show that 2D Fe_(1-x)S is a stable semiconductor with a narrow bandgap of60 meV.In addition to Fe_(1-x)S,the method is universal in growing various non-layered 2D TMCs containing ordered cation vacancies,including Fe_(1-x)Se,Co_(1-x)S,Cr_(1-x)S,and V_(1-x)S.This work paves the way to grow and exploit properties of non-layered materials at 2D thickness limit.
基金supported by the National Natural Science Foundation of China(Grant No.41305116)the National Basic Research Program of China(Grant No.2011CB403401)the Specific Team Fund of Chinese Academy of Meteorological Sciences(Grant No.2010Z002)
文摘As an important anthropogenic volatile organic compound(VOC), m-xylene has attracted numerous attentions due to its potential in secondary organic aerosol(SOA) formation. In this study, effects of aluminium dust seeds(boehmite and alumina) on SOA yield and aerosol size in m-xylene/NOx photo-oxidation were investigated in a 2 m3 smog chamber at 30°C and 50% relative humidity. Compared to the seed-free system, the presence of aluminium seeds resulted in an increase in the SOA yield, and also enhanced the O3 concentration in the chamber. The photolysis of O3 is a major source of OH radical, which is the most important oxidant of m-xylene. The increase in O3 concentration could result in the generation of more OH radicals, and finally contribute to the SOA formation. Seed particles influence the SOA size mainly by acting as condensation nuclei. Semi-volatile organic compounds(SVOCs) were condensed onto these nuclei, resulting in the increase in SOA size. However, when aluminium seeds with high concentrations were introduced into the system, SVOCs that had been condensed onto each particle were dispersed by these seeds, leading to the reduction in aerosol size.
基金supported by the National Natural Science Foundation of China (20873035)
文摘The thermodynamic properties of a binary self-condensing vinyl polymerization system consisting of monomers and inimers are investigated by the principle of statistical mechanics.In detail,in terms of two types of canonical partition functions constructed from different viewpoints,the equilibrium free energy,the law of mass action and the size distribution of hyperbranched polymers are obtained.As an application,the specific heat,equation of state and isothermal compressibility concerning the polymerization are given as well.To study the dimension of hyperbranched polymers in the system,a recursion formula satisfied by the(k+1)-th and k-th mean square radius of gyration is derived,and then the first,second and third radius of gyration under different solvent conditions are presented.The influences of the fraction of inimers,the conversion of vinyl groups and the solvent effect on the average dimension of hyperbranched polymers are discussed.