In this paper,a carbon based iridium (Ir) catalyst was prepared by an ion exchange procedure using H2IrCl6 as precursor and a strong basic anion exchange resin as substrate. The Ir/Carbon sample was obtained by carbon...In this paper,a carbon based iridium (Ir) catalyst was prepared by an ion exchange procedure using H2IrCl6 as precursor and a strong basic anion exchange resin as substrate. The Ir/Carbon sample was obtained by carbonizing the precursor. Effects of carbonization parameters such as temperature and time on size and dispersion of iridium crystallite were studied. Samples were prepared at 400 oC and 500 oC to investigate the effect of carbonization temperature. The SEM image of the Ir/Carbon composite shows a hard particle of 0. 2 - 0. 4 mm in diameter,which maintains a spherical shape. The TEM images of the catalyst show that no obvious effects of carbonization temperature or time are observed on the iridium particle size. Calcinated Ir nanoparticles prepared in ion exchange still keep their small particle-sized and narrow-sized distribution. The content of Ir supported on carbon can be well controlled simply by adjusting the relative ratio of Ir to carbon. Such a promising synthesis procedure is a versatile approach that can be extended to the fabrication of some carbon-supported metal catalysts or as a simple,rapid,and highly sensitive method.展开更多
In this paper, adsorption properties of dibenzothiophene (DBT) on carbon nanotube, carbon nanotube supported oxide state and sulfide state CoMo catalysts are studied by using thermal gravimetric analysis (TGA) techniq...In this paper, adsorption properties of dibenzothiophene (DBT) on carbon nanotube, carbon nanotube supported oxide state and sulfide state CoMo catalysts are studied by using thermal gravimetric analysis (TGA) technique and FT-IR spectroscopy. Activated carbon support, γ-AlgO3 support and supported CoMo catalysts are also subjected to studies for comparison. It was found that sulfide state CoMoS/MWCNT, CoMoS/AC and CoMoS/γ-Al2O3 catalysts adsorbed much more DBT molecules than their corresponding oxide state catalysts, as well as their corresponding supports. The chemically adsorbed DBT aromatic molecules did not undergo decomposition on the surface of supports, supported oxide state CoMo catalysts and sulfide state CoMo catalysts when out-gassing at 373 K. FT-IR results indicated that DBT molecules mainly stand upright on the active sites (acid sites and/or transition active phases) of CoMoS/MWCNT catalyst. However, DBT aromatic molecules mainly lie flat on MWCNT and CoMoO/MWCNT.展开更多
A Si-Al-lr oxidation resistant coating was prepared for SiC coated carbon/carbon composites by slurry dipping. The phase composition, microstructure and oxidation resistance of the as-prepared Si-Al-lr coating were st...A Si-Al-lr oxidation resistant coating was prepared for SiC coated carbon/carbon composites by slurry dipping. The phase composition, microstructure and oxidation resistance of the as-prepared Si-Al-lr coating were studied by XRD （X-ray diffraction）, SEM （scanning electron microscopy）, and isothermal oxidation test at 1773 K in air, respectively. The surface of the as-prepared Si-Al-lr coating was dense and the thickness was approximately 100 um. Its anti-oxidation property was superior to that of the inner SiC coating. The weight loss of SiC/Si- Al-lr coated carbon/carbon composites was less than 5 wt. pct after oxidation at 1773 K in air for 79 h. The local oxidation defects in the coating may result in the failure of the SiC/Si-Al-Ir coating.展开更多
利用低活性载体精确调控活性金属的电子结构是开发高性能电催化剂的有效途径,金属与载体之间高度灵活的电子相互作用可优化催化性能。在此,将Ir纳米团簇(Ir@NC)均匀地负载在氮掺杂炭框架上,制备了一种高效的析氢反应(HER)电催化剂。合...利用低活性载体精确调控活性金属的电子结构是开发高性能电催化剂的有效途径,金属与载体之间高度灵活的电子相互作用可优化催化性能。在此,将Ir纳米团簇(Ir@NC)均匀地负载在氮掺杂炭框架上,制备了一种高效的析氢反应(HER)电催化剂。合成过程是将在900℃下退火制备的沸石咪唑盐框架-8(ZIF-8)作为碳源浸入IrCl_(3)溶液中,然后在400℃的H_(2)/Ar气氛下进行煅烧还原处理。氮掺杂炭框架的三维多孔结构暴露了更多的活性金属位点,Ir簇和氮掺杂炭载体之间的协同效应有效地调节了Ir的电子结构,优化了HER过程。在酸性介质中,Ir@NC表现出显著的HER电催化活性:在10 mA cm^(-2)的条件下,过电位仅为23 mV,具有超低的Tafel斜率(25.8 mV dec^(-1)),且在10 mA cm^(-2)的条件下可稳定运行24 h以上。制备的电催化剂具有高活性、合成路线简便、可规模化制备等优点,有望成为一种极有前途的候选催化剂用于酸性水裂解进行工业制氢。展开更多
Light-induced infrared emission spectroscopy (LIRES) is a novel technique that permits to receive high-quality spectra in the mid-infrared region. Low-intensity visible light connected to a highly sensitive FTIR spect...Light-induced infrared emission spectroscopy (LIRES) is a novel technique that permits to receive high-quality spectra in the mid-infrared region. Low-intensity visible light connected to a highly sensitive FTIR spectrometer is more advantageous for studying any samples, including biological samples without any damage. This technique permits obtaining unique information on the molecule structure via vibrational excitation fundamental frequencies, overtones, and combination modes. It also enables a direct observation of vibrational radiation transitions in vibrationally excited molecules as well as the channels of vibration energy redistribution, which is not allowed with any other method. In this work, the LIRES is being tested as a technique for studying of vibrationally-excited molecules of carbon tetrachloride and benzene in the liquid phase. On the other hand, using transparent liquids, we had tried to understand some of the physical phenomena that can drive emission in mid-IR. The characteristics of the infrared emission of both liquid species produced by different wavelength radiation from various types of light systems (100 - watt Xe-lamp and Nd:YAG laser;lambda = 1064 nm (8 mW) and lambda = 532 nm (4 mW)) are presented. We demonstrated that the IR-signal, as well as spectral properties of carbon tetrachloride and benzene, was dependent on the wavelength and power of excitation beam. Results obtained with different light sources show that the visible light produces a nonlinear IR-emission signal in transparent liquids. We believe that the visible light is the source of the nonlinear response and is producing the vibration excitation as well as photostimulated transformations of the molecules possessing the high activity for the nonlinear response.展开更多
基金Sponsored by the National Natural Science Foundation of China(Grant No. 20806011)the Dalian Science and Technology Foundation of China(GrantNo. 2008A14GX240)
文摘In this paper,a carbon based iridium (Ir) catalyst was prepared by an ion exchange procedure using H2IrCl6 as precursor and a strong basic anion exchange resin as substrate. The Ir/Carbon sample was obtained by carbonizing the precursor. Effects of carbonization parameters such as temperature and time on size and dispersion of iridium crystallite were studied. Samples were prepared at 400 oC and 500 oC to investigate the effect of carbonization temperature. The SEM image of the Ir/Carbon composite shows a hard particle of 0. 2 - 0. 4 mm in diameter,which maintains a spherical shape. The TEM images of the catalyst show that no obvious effects of carbonization temperature or time are observed on the iridium particle size. Calcinated Ir nanoparticles prepared in ion exchange still keep their small particle-sized and narrow-sized distribution. The content of Ir supported on carbon can be well controlled simply by adjusting the relative ratio of Ir to carbon. Such a promising synthesis procedure is a versatile approach that can be extended to the fabrication of some carbon-supported metal catalysts or as a simple,rapid,and highly sensitive method.
基金Foundation of Innovation for Middle-aged and Youth, CNPC (Foundation No.W990411)
文摘In this paper, adsorption properties of dibenzothiophene (DBT) on carbon nanotube, carbon nanotube supported oxide state and sulfide state CoMo catalysts are studied by using thermal gravimetric analysis (TGA) technique and FT-IR spectroscopy. Activated carbon support, γ-AlgO3 support and supported CoMo catalysts are also subjected to studies for comparison. It was found that sulfide state CoMoS/MWCNT, CoMoS/AC and CoMoS/γ-Al2O3 catalysts adsorbed much more DBT molecules than their corresponding oxide state catalysts, as well as their corresponding supports. The chemically adsorbed DBT aromatic molecules did not undergo decomposition on the surface of supports, supported oxide state CoMo catalysts and sulfide state CoMo catalysts when out-gassing at 373 K. FT-IR results indicated that DBT molecules mainly stand upright on the active sites (acid sites and/or transition active phases) of CoMoS/MWCNT catalyst. However, DBT aromatic molecules mainly lie flat on MWCNT and CoMoO/MWCNT.
基金supported by the National "973"Project under grant No. 2006CB600908
文摘A Si-Al-lr oxidation resistant coating was prepared for SiC coated carbon/carbon composites by slurry dipping. The phase composition, microstructure and oxidation resistance of the as-prepared Si-Al-lr coating were studied by XRD （X-ray diffraction）, SEM （scanning electron microscopy）, and isothermal oxidation test at 1773 K in air, respectively. The surface of the as-prepared Si-Al-lr coating was dense and the thickness was approximately 100 um. Its anti-oxidation property was superior to that of the inner SiC coating. The weight loss of SiC/Si- Al-lr coated carbon/carbon composites was less than 5 wt. pct after oxidation at 1773 K in air for 79 h. The local oxidation defects in the coating may result in the failure of the SiC/Si-Al-Ir coating.
文摘利用低活性载体精确调控活性金属的电子结构是开发高性能电催化剂的有效途径,金属与载体之间高度灵活的电子相互作用可优化催化性能。在此,将Ir纳米团簇(Ir@NC)均匀地负载在氮掺杂炭框架上,制备了一种高效的析氢反应(HER)电催化剂。合成过程是将在900℃下退火制备的沸石咪唑盐框架-8(ZIF-8)作为碳源浸入IrCl_(3)溶液中,然后在400℃的H_(2)/Ar气氛下进行煅烧还原处理。氮掺杂炭框架的三维多孔结构暴露了更多的活性金属位点,Ir簇和氮掺杂炭载体之间的协同效应有效地调节了Ir的电子结构,优化了HER过程。在酸性介质中,Ir@NC表现出显著的HER电催化活性:在10 mA cm^(-2)的条件下,过电位仅为23 mV,具有超低的Tafel斜率(25.8 mV dec^(-1)),且在10 mA cm^(-2)的条件下可稳定运行24 h以上。制备的电催化剂具有高活性、合成路线简便、可规模化制备等优点,有望成为一种极有前途的候选催化剂用于酸性水裂解进行工业制氢。
文摘Light-induced infrared emission spectroscopy (LIRES) is a novel technique that permits to receive high-quality spectra in the mid-infrared region. Low-intensity visible light connected to a highly sensitive FTIR spectrometer is more advantageous for studying any samples, including biological samples without any damage. This technique permits obtaining unique information on the molecule structure via vibrational excitation fundamental frequencies, overtones, and combination modes. It also enables a direct observation of vibrational radiation transitions in vibrationally excited molecules as well as the channels of vibration energy redistribution, which is not allowed with any other method. In this work, the LIRES is being tested as a technique for studying of vibrationally-excited molecules of carbon tetrachloride and benzene in the liquid phase. On the other hand, using transparent liquids, we had tried to understand some of the physical phenomena that can drive emission in mid-IR. The characteristics of the infrared emission of both liquid species produced by different wavelength radiation from various types of light systems (100 - watt Xe-lamp and Nd:YAG laser;lambda = 1064 nm (8 mW) and lambda = 532 nm (4 mW)) are presented. We demonstrated that the IR-signal, as well as spectral properties of carbon tetrachloride and benzene, was dependent on the wavelength and power of excitation beam. Results obtained with different light sources show that the visible light produces a nonlinear IR-emission signal in transparent liquids. We believe that the visible light is the source of the nonlinear response and is producing the vibration excitation as well as photostimulated transformations of the molecules possessing the high activity for the nonlinear response.
