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费-托合成铁催化剂中金属与担体相互作用的考察

INVESTIGATION OF METAL-SUPPORTINTERACTION(MSI) OF FISCHER-TROPSCH IRON CATALYSTS

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【作者】 王承玉章素蔡海林潘立金梁东白林励吾

【Author】 Wang Chengyu Zhang Su Cai Hailin Pan Lijin Liang Dongbai Lin Liwu(Dalian Institute of Chemical Physics, Academia Sciences, Dalian)

【机构】 中国科学院大连化学物理研究所中国科学院大连化学物理研究所 大连大连大连

【摘要】 将费-托合成铁催化剂Fe/Al2O3和Fe/SiO2在空气中经一系列温度(25、120、480、650、780和1000℃)予处理并在相同条件(H2、480℃、4h)下还原,然后作原位穆斯堡尔谱和高分辨电镜的考察,结果表明,在较低温度下予处理时,随着予处理温度的升高,Fe/Al2O3和Fe/SiO2中的铁被还原为Fe(O)的量增加,但当达到某一温度(Fe/Al2O3为650℃、Fe/SiO2为480℃)时出现了转折,即随着予处理温度的增加,Fe(O)%降低,意味着MSI由原来的减弱变为增强。在较低的予处理温度时,生成了难以还原的铝酸铁盐和硅酸铁盐,使MSI效应为主。适当增强MSI对提高低碳烯烃选择性有利。

【Abstract】 Fischer-Tropsch iron catalysts Fe/Al2O3 and Fe/SiO2 which were pretreated in air at different temperatures (25℃,120℃,480℃,650℃, 780℃ and 1000℃) for 4h following reduction under the same conditions (H2, 450℃, 4 h) have been studied by in-situ Mossbauer spectroscopy and highresolution electron microscopy. The results show that the percentage of Fe(0) in Fe/Al2O3 and Fe/SiO2 passes through maxima at pretreatment temperatures of 650℃ and 480℃ respectively. It is ascribed to the possibility that when pretreating the samples at temperatures below the turninf points the increase in particle sizes of Fe2O3 which favors its reduction to iron metal, predominates over the increase in MSI for both Fe/Al2O3 and Fe/SiO2, while the contrary occurs at higher pretreatment temperatures.The maximum of Fe(0)% formation (or the minimum of MSI) occurs at pretreatment temperatures of 650℃ and 480℃ for Fe/Al2O3 and Fe/SiO2 respectively.MSI which is attributed to the formation of stable Fe (Ⅲ) species (Fe(Ⅲ) aluminate and Fe(Ⅲ)silicate, has been found to influence the selectivity of F-T reactions.

  • 【文献出处】 燃料化学学报 ,Journal of Fuel Chemistry and Technology , 编辑部邮箱 ,1989年02期
  • 【被引频次】2
  • 【下载频次】70
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