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氧化镍与载体相互作用对乙烷氧化脱氢的影响

Investigation of the Interaction between NiO and Support,γ-Al2O3, for Oxidative Dehydrogenation of Ethane

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【作者】 陈铜李文钊于春英

【Author】 Chen Tong; Li Wenzhao;YU Cjunying (Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 )

【机构】 中国科学院大连化学物理研究所!大连116023

【摘要】 研究了担载型催化剂NiO/γ-Al2O3的乙烷氧化脱氧(ODHE)性能,发现在400-500℃的考察温区内,担载型NiO较纯NiO的乙烯选择性有较大提高,保持在80%~90%之间,其中含17%Ni的样品500℃时乙烷的转化率为31%,乙烯选择性达82%.XRD、H2-TPR及原位磁测量结果表明:催化剂的活性相是与载体相互作用较小的、处于表层的微晶态NiO,NiO中非化学计量氧仍为活性氧物种.催化剂焙烧温度的提高,一方面降低了活性相中非化学计量氧量,同时加剧了NiO与载体γ-Al2O3的相互作用,二者均使活性降低.O2-TPD研究表明:与纯NiO相比,在Nio/γ-Al2O3中,其非化学计量氧的脱附温度发生变化,其中,α氧脱附温度向低温移动约50℃,而对乙烯选择性有关的β氧的脱出则向高温区移动了约200℃,正好与反应温区对应,进一步证实非化学计量氧与ODHE反应之间存在对应关系,上述结果表明那些对氧化镍还原有一定的阻碍作用,尤其阻碍镍深度还原(Ni2+→Nio)的载体对促进反应的乙烯选择性是有利的.

【Abstract】 The catalytic behavior of alumina-supported NiO catalysts for oxidative dehydrogenation of ethane (ODHE) has been inveshgated in the temperature range of 400~ 500℃ A much better improvement of selectivity towards ethylene can be observed, i e. the selectivity of 82% ~ 92% for ethylene can be maintained. The optimum yield of ethylene of 25. 3% is obtained over 17% NiO/γ-Al2O3 at 500℃. It is suggested that the NiO of non MSSI(Metal-support strong interation)is the active phase and the nonstoichiometric oxygen in NiO lattice is the active oxygen species for ODHE. Comparing the O2-TPD spectra of NiO with NiO/γ-Al2O3, the high selechvity fot ethylene over the alumina-supported NiO catalysts can be explained.

  • 【文献出处】 物理化学学报 ,ACTA PHYSICO-CHIMICA SINICA , 编辑部邮箱 ,1999年07期
  • 【分类号】O643
  • 【被引频次】22
  • 【下载频次】201
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