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      • Pd' Location and Adsorbate Interactions in PdH-SAPO-34-studied by EPR and Electron Spin-Echo Modulation Spectroscopies

        Yu,Jong-Sung,Larry Kevan,Vadim Kurshev,Back,Gern-Ho 國立昌原大學校 基礎科學硏究所 1994 基礎科學硏究所論文集 Vol.6 No.-

        EPR and electron spin-echo modulation (ESEM) spectroscopies have been used to monitor the location of Pd' and its interaction with water, methanol, ethanol, ethene, benzene, carbon monoxide and ammonia in silicoaluminophosphate type 34(SAPO-34) molecular sieve containing Pd'' by ion exchange. After activation at 600℃, three different Pb' species are observed: A₁(g1=2,177), A₂(g1=2.136) and A₃(g1=2,070) with a common gⅡ=2.92. These correspond to three different site locations in the framework. A₁is assigned to the least accessible site Ⅲ in the centre of a hexagonal prism. A₃ to site I displaced from a six-ring into the ellipsoidal cage and A₂ to the most accessible site Ⅳ near an eight-ring window based on adsorption of oxygen and hydrogen and 31P modulations from the SAPO framework observed by ESEM. Oxygen and water oxidize Pd' ions in an activated sample to Pd'' ions complexed to O₂-, indicating water decomposition. Adsorption of methanol and ethanol causes a change in the EPR spectrum which indicates some relocation of Pd'to allow better coordination with one molecule of the alcohol. Exposure to ethene also changes the EPR spectrum, indicating interaction of Pd' with it. ESEM shows that the Pd' species coordinates to one ethene molecule. The adsorption of carbon monoxide results in a Pd' complex with three molecules of carbon monoxide based on resolved 13C superhyperfine splittings. Upon adsorption of ammonia, one molecule of ammonia coordinates to Pd' based on resolved nitrogen hyperfine coupling.

      • Pd^(1) Location and Adsorbate Interactions in PdH-SAPO-34 studied by EPR and Electron Spin-Echo Modulation Spectroscopies

        Back, Gern-Ho,Yu, Jong-Sung,Vadim Kurshev,Larry Kevan 國立 昌原大學校 基礎科學硏究所 1994 基礎科學硏究所論文集 Vol.6 No.-

        EPR and electron spin-echo modulation (ESEM) spectroscopies have been used to monitor the location of Pd_(II) and its interaction with water, methanol, ethanol, ethene, benzene, carbon monoxide and ammonia in silicoaluminophosiphate type 34 (SAPO-34) molecular sieve containing Pd(II) by ion exchange. After activation at 600℃, three different Pd' species are observed: A_(1)(g_(⊥) = 2.177), A_(2)(g_(⊥) = 2.136) and A_(3)(g_(⊥) = 2.070) with a common g_(Ⅱ)= 2.92. These correspond to three different site locations in the framework. A_(1) is assigned to the least accessible site Ⅲ in the centre of a hexagonal prism, A_(3) to site I displaced from a six-ring into the ellipsoidal cage and A_(2) to the most accessible site Ⅳ near an eight-ring window based on adsorption of oxygen and hydrogen and ^(31)P modulations from the SAPO framework observed by ESEM. Oxygen and water oxidize Pd_(I) lons in an activated sample to Pd^(Ⅱ) ions complexed to O_(2)^(-), indicating water decomposition. Adsorption of methanol and ethanol causes a change in the EPR spectrum which indicates some relocation of Pd^(Ⅰ) to allow better coordination with one molecule of the alcohol. Exposure to ethene also changes the EPR spectrum, indicating interaction of Pd^(Ⅰ) with it. ESEM shows that the Pd^(Ⅰ) species coordinates to one ethene molecule. The adsorption of carbon monoxide results in a Pd^(Ⅰ) complex with three molecules of carbon monoxide based on resolved ^(13)C superhyperfine splittings. Upon adsorption of ammonia, one molecule of ammonia coordinates to Pd^(Ⅰ) based on resolved nitrogen hyperfine coupling.

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