Simultaneously controlling the size of Au nanoparticles and immobilizing their location to specific active sites while hindering migration and sintering at elevated temperatures is a current challenge within materials...Simultaneously controlling the size of Au nanoparticles and immobilizing their location to specific active sites while hindering migration and sintering at elevated temperatures is a current challenge within materials chemistry.Typical methods require the use of protecting agents to control the properties of Au nanoparticles and therefore it is difficult to decouple the influence of the protecting agent and the support material.By functionalizing the internal surface area of mesoporous carbon supports with thiol groups and implementing a simple acid extraction step,we are able to design the resulting materials with precise control over the Au nanoparticle size without the need for the presence of any protecting group,whilst simultaneously confining the nanoparticles to within the internal porous network.Monodispersed Au nanoparticles in the absence of protecting agents were encapsulated into ordered mesoporous carbon at various loading levels via a coordination-assisted self-assembly approach.The X-ray diffractograms and transmission electron microscopy micrographs show that the particles have controlled and well-defined diameters between 3 and 18 nm at concentrations between 1.1 and 9.0 wt%.The Au nanoparticles are intercalated into the pore matrix to different degrees depending on the synthesis conditions and are stable after high temperature treatment at 600 °C.N2 adsorption-desorption isotherms show that the Au functionalized mesoporous carbon catalysts possess high surface areas(1269–1743 m^2/g),large pore volumes(0.78–1.38 cm^3/g)and interpenetrated,uniform bimodal mesopores with the primary larger mesopore lying in the range of 3.4–5.7 nm and the smaller secondary mesopore having a diameter close to 2 nm.X-ray absorption near extended spectroscopy analysis reveals changes to the electronic properties of the Au nanoparticles as a function of reduced particle size.The predominant factors that significantly determine the end Au nanoparticle size is both the thiol group concentration and subjecting the as-made materials to an additional concentrated sulfuric acid extraction step.展开更多
Information on the palaeoenvironm ent from Late Pleistocene to Holocen e in northwestern Yannan Plateau has been deduced from a study of a 28.81m-long core taken from Napahai Lake.The results from Relative Brightness ...Information on the palaeoenvironm ent from Late Pleistocene to Holocen e in northwestern Yannan Plateau has been deduced from a study of a 28.81m-long core taken from Napahai Lake.The results from Relative Brightness In-dex(RBI )as well as those from the lithological analyses of bulk sediments,total organic carbon and granulometric analy-ses have been used to reconstruct the environmental and climatic evoluti on of the area.The ages were provided by three 14 C datings.The record suggested a climate fluctuation between warm-dry a nd cool-wet from ca.57to 32ka B.P.,which led a shallowing and swamping of the l ake.The water level again increased quickly at ca.32ka B.P.,reached it’ s peak during LGM(Last Glacial Maximum,ca.18-20ka B.P.)and remained relative high until ca.15ka B.P.The high wa-ter level at LGM is attributed to cold-wet conditions.The area experienced an abrupt and unstable climatic ch anges dur-ing the transition period from15to 10ka B.P.with a dominated littoral en vironment.Awarm-dry climate led to the contrac-tion of the lake during the Holocene a nd reed-swamps became dominant.After a minor wet-cool pulse during the L ate Holocene,the modern climate became to be established.展开更多
High-temperature creep properties of sintered uranium dioxide pellets with two grain sizes (9.0 μm and 23.8μm) were studied. The results indicate that the creep rate becomes a little faster with the reduction of t...High-temperature creep properties of sintered uranium dioxide pellets with two grain sizes (9.0 μm and 23.8μm) were studied. The results indicate that the creep rate becomes a little faster with the reduction of the uranium dioxide grain size at the same temperature and the same load. At the same temperature, the logarithmic value of the steady creep rate vs stress has linear relation, and with increasing load, the steady creep rate of the sintered uranium dioxide pellet increases. Under the same load, the steady creep rate of the sintered uranium dioxide pellet increases with increasing temperature; and the creep rates of sintered uranium dioxide pellet with the grain size of 9.0 μm and 23.8 μm under 10 MPa are almost the same. The creep process is controlled both by Nabarro--Herring creep and Hamper-Dorn creep for uranium dioxide pellet with grain size of 9.0 μm, while Hamper---Dora creep is the dominantmechanism for uranium dioxide with grain size of 23.8 μm.展开更多
Porous medium has an obvious effect on the formation of carbon dioxide hydrate. In order to study the characteristics of CO2 hydrate formation in porous medium below the freezing point, the experiment of CO2 hydrate f...Porous medium has an obvious effect on the formation of carbon dioxide hydrate. In order to study the characteristics of CO2 hydrate formation in porous medium below the freezing point, the experiment of CO2 hydrate formation was conducted in a high-pressure 1.8-L cell in the presence of porous media with a particle size of 380 μm, 500 μm and 700 μm, respectively. The test results showed that the porous medium had an important influence on the process of CO2 hydrate formation below the freezing point. Compared with porous media with a particle size of 500 μm and 700 μm, respectively, the average hydrate formation rate and gas storage capacity of carbon dioxide hydrate in the porous medium with a particle size of 380 μm attained 0.016 14 mol/h and 65.094 L/L, respectively. The results also indicated that, within a certain range of particle sizes, the smaller the particle size of porous medium was, the larger the average hydrate formation rate and the gas storage capacity of CO2 hydrate during the process of hydrate formation would be.展开更多
基金supported by the State Key Basic Research Program of China(2013CB934102)the National Natural Science Foundation of China(21322308,21173149)+2 种基金the Program for Changjiang Scholars and Innovative Research Team in University(PCSIRT-IRT1269)the Research Fund for the Doctoral Program of Higher Education(20123127110004)Shanghai Science&Technology and Education Committee(11JC1409200,DZL123,S30406)~~
文摘Simultaneously controlling the size of Au nanoparticles and immobilizing their location to specific active sites while hindering migration and sintering at elevated temperatures is a current challenge within materials chemistry.Typical methods require the use of protecting agents to control the properties of Au nanoparticles and therefore it is difficult to decouple the influence of the protecting agent and the support material.By functionalizing the internal surface area of mesoporous carbon supports with thiol groups and implementing a simple acid extraction step,we are able to design the resulting materials with precise control over the Au nanoparticle size without the need for the presence of any protecting group,whilst simultaneously confining the nanoparticles to within the internal porous network.Monodispersed Au nanoparticles in the absence of protecting agents were encapsulated into ordered mesoporous carbon at various loading levels via a coordination-assisted self-assembly approach.The X-ray diffractograms and transmission electron microscopy micrographs show that the particles have controlled and well-defined diameters between 3 and 18 nm at concentrations between 1.1 and 9.0 wt%.The Au nanoparticles are intercalated into the pore matrix to different degrees depending on the synthesis conditions and are stable after high temperature treatment at 600 °C.N2 adsorption-desorption isotherms show that the Au functionalized mesoporous carbon catalysts possess high surface areas(1269–1743 m^2/g),large pore volumes(0.78–1.38 cm^3/g)and interpenetrated,uniform bimodal mesopores with the primary larger mesopore lying in the range of 3.4–5.7 nm and the smaller secondary mesopore having a diameter close to 2 nm.X-ray absorption near extended spectroscopy analysis reveals changes to the electronic properties of the Au nanoparticles as a function of reduced particle size.The predominant factors that significantly determine the end Au nanoparticle size is both the thiol group concentration and subjecting the as-made materials to an additional concentrated sulfuric acid extraction step.
文摘Information on the palaeoenvironm ent from Late Pleistocene to Holocen e in northwestern Yannan Plateau has been deduced from a study of a 28.81m-long core taken from Napahai Lake.The results from Relative Brightness In-dex(RBI )as well as those from the lithological analyses of bulk sediments,total organic carbon and granulometric analy-ses have been used to reconstruct the environmental and climatic evoluti on of the area.The ages were provided by three 14 C datings.The record suggested a climate fluctuation between warm-dry a nd cool-wet from ca.57to 32ka B.P.,which led a shallowing and swamping of the l ake.The water level again increased quickly at ca.32ka B.P.,reached it’ s peak during LGM(Last Glacial Maximum,ca.18-20ka B.P.)and remained relative high until ca.15ka B.P.The high wa-ter level at LGM is attributed to cold-wet conditions.The area experienced an abrupt and unstable climatic ch anges dur-ing the transition period from15to 10ka B.P.with a dominated littoral en vironment.Awarm-dry climate led to the contrac-tion of the lake during the Holocene a nd reed-swamps became dominant.After a minor wet-cool pulse during the L ate Holocene,the modern climate became to be established.
基金Project(50874126)supported by the National Natural Science Foundation of China
文摘High-temperature creep properties of sintered uranium dioxide pellets with two grain sizes (9.0 μm and 23.8μm) were studied. The results indicate that the creep rate becomes a little faster with the reduction of the uranium dioxide grain size at the same temperature and the same load. At the same temperature, the logarithmic value of the steady creep rate vs stress has linear relation, and with increasing load, the steady creep rate of the sintered uranium dioxide pellet increases. Under the same load, the steady creep rate of the sintered uranium dioxide pellet increases with increasing temperature; and the creep rates of sintered uranium dioxide pellet with the grain size of 9.0 μm and 23.8 μm under 10 MPa are almost the same. The creep process is controlled both by Nabarro--Herring creep and Hamper-Dorn creep for uranium dioxide pellet with grain size of 9.0 μm, while Hamper---Dora creep is the dominantmechanism for uranium dioxide with grain size of 23.8 μm.
基金financially supported by the Natural Science Foundation of China (No. 51266005)the Science and Technology Research Key Project of the Ministry of Education (No. 1106ZBB007)+1 种基金the Hongliu Outstanding Talent Program of LUT (No. Q201101)the Open Fund of Natural Gas Hydrate Key Laboratory, Chinese Academy of Sciences (No. y007s3)
文摘Porous medium has an obvious effect on the formation of carbon dioxide hydrate. In order to study the characteristics of CO2 hydrate formation in porous medium below the freezing point, the experiment of CO2 hydrate formation was conducted in a high-pressure 1.8-L cell in the presence of porous media with a particle size of 380 μm, 500 μm and 700 μm, respectively. The test results showed that the porous medium had an important influence on the process of CO2 hydrate formation below the freezing point. Compared with porous media with a particle size of 500 μm and 700 μm, respectively, the average hydrate formation rate and gas storage capacity of carbon dioxide hydrate in the porous medium with a particle size of 380 μm attained 0.016 14 mol/h and 65.094 L/L, respectively. The results also indicated that, within a certain range of particle sizes, the smaller the particle size of porous medium was, the larger the average hydrate formation rate and the gas storage capacity of CO2 hydrate during the process of hydrate formation would be.