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作 者:刘振林[1] 孟明[1] 伏义路[1] 李春林[1] 姜明[1] 胡天斗[2] 谢亚宁[2]
机构地区:[1]中国科学技术大学化学物理系,安徽合肥230026 [2]中国科学院高能物理研究所,北京100039
出 处:《分子催化》2002年第1期25-30,共6页Journal of Molecular Catalysis(China)
基 金:国家自然科学基金资助项目 ( No.2 98730 44); BSRF重点课题资助项目
摘 要:采用氨气还原法制备了 Na Y分子筛负载的 Mo Co/ Y、Mo Ni/ Y双组分氮化物催化剂 ,用 XRD和 EXAFS方法表征了样品的结构 ,并测定了其在 CH4+CO2 重整反应中的活性 .在氧化态时 ,Mo Co/ Y样品中主要存在Co Mo O4和 Co3O4两种物相 ,Mo的配位状态接近于 Co Mo O4,而 Co的配位状态更接近于 Co3O4.Mo Ni/ Y样品中主要有 Ni Mo O4和 Ni O两种物相 ,Mo的配位状态接近于 Ni Mo O4,而 Ni的配位状态可能是 Ni Mo O4和 Ni O两种化合物中 Ni配位状态的平均效果 .Ni- Mo之间的相互作用似乎比 Co- Mo相对较强 .在氮化态时 ,两种样品中Mo的配位状态较为相似 ,但既不同于 Mo O3,也不同于单组分 γ- Mo2 N.Co和 Ni的配位状态都不同于各自在氧化态下的状态 ,且都在相同的位置出现一个新强峰 .这似乎表明 Mo Co和 Mo Ni生成了结构相似的氮化物 .在CH4+CO2 重整反应中 ,氮化态 Mo Co/ Y和 Mo Ni/ Y的活性大大超过非负载单组分 γ- Mo2 N催化剂 .其中 Mo Ni/Y的活性相对更好一些 ,且活性随MoCo/ Y and MoNi/ Y bicomponent nitrides catalysts were prepared by temperature\|programmed reduction in NH\-3. Structure of samples was characterized by XRD and EXAFS methods. Samples underwent activity test in CH\-4+CO\-2 reforming reaction. CoMoO\-4 and Co\-3O\-4 exist on oxidic MoCo/ Y . The coordination environment of Mo is close to Mo in CoMoO\-4, and Co atom has similar coordination environment as Co in Co\-3O\-4. Two species, NiMoO\-4 and NiO, are on oxidic MoNi/ Y . The coordination environment of Mo is close to Mo in NiMoO\-4, and the coordination environment of Ni atom seems to be a mixed results of Ni in NiMoO\-4 and NiO. Interaction between Ni and Mo is likely stronger than that between Co and Mo. After nitridation, the coordination environment of Mo is similar for these two samples, but different from MoO\-3 and γ \|Mo\-2N. Ni and Co atom have different coordination environments from their oxidic state, and show a new strong peak at the same position. This seems to indicate that MoCo and MoNi form nitrides with similar structure. In CH\-4+CO\-2 reforming reaction, the activities of MoCo/ Y and MoNi/ Y nitrides are higher than unsupported γ \|Mo\-2N, and MoNi/ Y is even better. The activity of MoNi/ Y increases with the Ni loading.
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