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金属有机骨架材料Fe-MIL-100诱导的铁基费托催化剂的合成及催化性能研究
  • ISSN号:0567-7351
  • 期刊名称:《化学学报》
  • 时间:0
  • 分类:TQ223.121[化学工程—有机化工]
  • 作者机构:[1]中国石油大学华东化学工程学院,青岛266000, [2]中科合成油技术有限公司煤炭间接液化国家工程实验室,北京101407, [3]中国科学院山西煤炭化学研究所煤转化国家重点实验室,太原030001
  • 相关基金:国家自然科学基金重大研究计划项目(No.91545109); 山西省国际科技合作项目(No.2014081004)资助~~
中文摘要:

随着石油资源的日益枯竭及环保要求的日益严苛,寻找非石油路线生产清洁燃料的方法迫在眉睫,费-托合成是一种以合成气(CO和H_2)为原料生产液体燃料的高效方法.铁基费-托合成催化剂广泛应用于工业,本工作研究了多孔碳材料包裹的活性组分高度分散的铁基费托催化剂的制备、结构及费-托合成反应性能.以金属有机骨架材料Fe-MIL-100为前驱体,通过控制碳化温度调节催化剂金属负载量、催化剂粒子尺寸及铁的相态.研究发现碳化温度为500℃所得催化剂在反应温度为260℃、压力为3 MPa、空速为8000 h~(-1)时CO转化率达到68%,展现出优良的中温费托合成反应性能.

英文摘要:

Depletion of crude oil resources and environmental concerns have spurred worldwide interest in finding un-oil route for liquid fuels. Fischer-Tropsch synthesis is an effective progress for a wide spectrum of hydrocarbon chains from synthesis gas. The use of iron-based catalysts would be preferred in the industry. Here we present a strategy to produce highly dispersed active component embedded in a matrix of porous carbon. Through the carbonization of iron-containing metal- organic frameworks (Fe-MIL-100) at different temperature in N2, four kinds of Fe@C catalysts were prepared. Glucose was used as additional carbon precursor for the synthesis catalyst samples to prevent particle agglomeration. Our strategy avoids the particle agglomeration in the weak metal-support interaction Fe@C catalysts during calcination, reduction and reaction. The structure and morphology of prepared catalysts were characterized by X-ray diffraction (XRD), N2 physical adsorption, transmission electron microscopy (TEM), inductively coupled plasma-atomic emission spectrometer (ICP-AES). It is demon- strated that the iron loading, the particle size, and the Fe phase structure of Fe@C catalysts can be controlled by changing the carbonization temperature of Fe-MIL-100. With increasing the temperature, the iron loading and the particle size increase gradually. Depending on the carbonization temperature, the Fe3O4 phase is dominant at 400 and 500 ℃. The FeO and Fe phase appear at 600 ℃. The Fe3C phase prevails at 700℃. The high dispersion of the metal phase and its encapsulation in a highly porous carbon matrix result in an unrivalled FTS activity. The spatial restriction created by encapsulation seems to minimize sintering and oxidation of the active Hagg carbide phase. When the reaction conditions were set at 260 ℃, 3 MPa, the space velocity of 8000 h-1, the conversion of CO is up to 68%. The Fe time yield (FTY) of the Fe@C-500 catalyst were as high as 164 μmolCO.gFe-1.s-1, which surpasses that of most F-T catalys

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期刊信息
  • 《化学学报》
  • 北大核心期刊(2014版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院上海有机化学研究所
  • 主编:周其林
  • 地址:上海市零陵路345号
  • 邮编:200032
  • 邮箱:hxxb@sioc.ac.cn
  • 电话:021-54925085
  • 国际标准刊号:ISSN:0567-7351
  • 国内统一刊号:ISSN:31-1320/O6
  • 邮发代号:4-209
  • 获奖情况:
  • 首届国家期刊奖,第二届国家期刊奖提名奖,中国期刊方阵“双高期刊”
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:28694