正己烷芳构化Zn、Ga分子筛催化剂的合成

IF 0.6 4区 工程技术 Q4 ENERGY & FUELS
Hiroyuki Imai, Maika Takada, Y. Ike
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引用次数: 0

摘要

乙烷、丙烷、正己烷等轻烷烃的芳构化是生产高附加值芳香族化合物尤其是苯、甲苯和二甲苯(BTX)的重要工艺,因为芳构化工艺可以适应使用天然气,以满足近几十年来石油化工行业对原料化学品日益增长的需求。在烷烃芳构化反应中,以ZSM-51 ~14、MCM-2215、ZSM-1116、L型沸石17 ~21为主要载体的载金属沸石催化剂得到了广泛的开发。特别是含Znor ga的ZSM-5分子筛,由于金属的脱氢作用和ZSM-5分子筛的Brønsted酸性(1),3),5),6),10),对芳香族化合物具有较高的催化活性和选择性。此外,通过离子交换和还原氧化处理将ZSM-5上的质子替换为金属种,以提供阳离子金属种等活性位点,而不是大块ZnO和Ga2O322)~25),金属种在ZSM-5上高度分散。由于烷烃的芳构化基本上是通过烷烃的脱氢进行的,因此增加活性金属位的数量对于提高催化性能非常重要。通过水热合成将金属种引入沸石骨架中,导致沸石中形成高度分散和隔离的金属种。此外,在沸石骨架中掺入三价Ga而不是Al会产生Brønsted酸位,其酸性比掺入Al所产生的酸位更弱(24),从而形成双功能烷烃芳构化催化剂(26)~30)。我们之前发现,水热法合成的含锌MFI沸石在不含Al的情况下,对正丁烷脱氢生成1,3-丁二烯具有较高的催化活性(31)。在沸石中引入Zn可以形成具有高脱氢活性的独立活性Zn位。因此,预计沸石中Zn和Ga分离位点的形成将提高沸石催化剂对烷烃芳构化(脱氢环化)选择性生成BTX的催化性能。这里我们报道直接合成mfi型零[研究说明]
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Synthesis of Zeolite Catalysts Containing Zn and Ga for Aromatization of n-Hexane
The aromatization of light alkanes including ethane, propane, and n-hexane is an important process for producing value-added aromatic compounds, especially benzene, toluene, and xylenes (BTX), because the aromatization process can be adapted to use natural gas, to meet the increased demands for raw chemicals in the petrochemical industry in recent decades. For the aromatization of alkanes, various metal-loaded zeolite catalysts based on ZSM-51)~14), MCM-2215), ZSM-1116), and L zeolite17)~21) have been extensively developed. In particular, Znor Ga-containing ZSM-5 provides high catalytic activities and selectivities for aromatic compounds because of the combination of the dehydrogenation over the metal species and Brønsted acidity of the ZSM-5 zeolite1),3),5),6),10). Furthermore, the metal species are highly dispersed on ZSM-5 through the replacement of protons on ZSM-5 with the metal species by ion exchange and reducing-oxidizing treatment to provide active sites such as cationic metal species instead of bulk ZnO and Ga2O322)~25). Since the aromatization of alkanes fundamentally proceeds via the dehydrogenation of alkanes, it is important to increase the number of active metal sites for improving the catalytic performances. The incorporation of metal species into the framework of zeolite through the hydrothermal synthesis leads to the formation of highly dispersed and isolated metal species in the zeolite. In addition, the incorporation of trivalent Ga species, instead of Al species, into the zeolite framework generates Brønsted acid sites with weaker acidity than those generated by the incorporation of Al species24), resulting in a bifunctional catalyst for the aromatization of alkanes26)~30). We previously found that Zn-containing MFI zeolite synthesized by the hydrothermal treatment in the absence of Al species exhibited a high catalytic activity for the dehydrogenation of n-butane to produce 1,3-butadiene31). Introducing Zn species into the zeolite would form isolated active Zn sites with high dehydrogenation activity. Therefore, it is expected that the formation of both isolated Zn and Ga sites in zeolite would improve the catalytic performances of zeolite catalysts for the aromatization (dehydrocyclization) of alkanes to selectively produce BTX. Here we report the direct synthesis of MFI-type zeo[Research Note]
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来源期刊
Journal of The Japan Petroleum Institute
Journal of The Japan Petroleum Institute 工程技术-工程:石油
CiteScore
1.70
自引率
10.00%
发文量
29
审稿时长
>12 weeks
期刊介绍: “Journal of the Japan Petroleum Institute”publishes articles on petroleum exploration, petroleum refining, petrochemicals and relevant subjects (such as natural gas, coal and so on). Papers published in this journal are also put out as the electronic journal editions on the web. Topics may range from fundamentals to applications. The latter may deal with a variety of subjects, such as: case studies in the development of oil fields, design and operational data of industrial processes, performances of commercial products and others
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