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Search for solid acid catalysts aiming at the development of bifunctional tandem catalysts for the one-pass synthesis of lower olefins via CO_2 hydrogenation

机译:搜索旨在通过CO_2氢化进行双烯烃一次通过合成的双官能串联催化剂的固体酸催化剂

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摘要

The development of methodologies for CO2 utilization is in high demand worldwide. Here, we propose bifunctional tandem catalysts of ZnZrOx (for CO2-to-methanol hydrogenation) and a series of solid acid catalysts (for subsequent methanol conversion to light olefins). As solid acid catalysts, we used zeolites and silicoaluminophosphates with different topologies, MOR, FER, MFI, *BEA, CHA, and ERI, confirmed by X-ray diffraction, electron microscopy, and nitrogen adsorption-desorption. They also showed the corresponding acid properties examined by ammonia adsorption. The tandem catalysts realized a one-pass synthesis of lower olefins, while no hydrocarbons were obtained using ZnZrOx only. According to the reaction test and ammonia adsorption, there seems to be no correlation between product yields and acid strength. The pore sizes and channel dimensionality of zeolites influence the selectivity of products; zeolites with small pores, such as MOR, SAPO34 and ERI, are promising, while zeolites with larger pores, such as MFI, produce heavier hydrocarbons. The results provide new insight into the design of innovative catalysts for CO2 utilization. (c) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:二氧化碳利用方法的开发在全球需求很大。在此,我们提出了Znzrox(用于CO 2 - 甲醇氢化)的双官能串联催化剂和一系列固体酸催化剂(用于随后的甲醇转化为光烯烃)。作为固体酸催化剂,我们使用沸石和硅铝磷酸酯,用不同的拓扑,MOR,FER,MFI,* BEA,CHA和ERI,通过X射线衍射,电子显微镜和氮吸附 - 解吸证实。他们还显示出通过氨吸附检查的相应酸性。串联催化剂实现了下烯烃的一次通过合成,而仅使用ZnZrox获得烃。根据反应试验和氨吸附,产率和酸强度之间似乎没有相关性。沸石的孔径和通道维度影响了产品的选择性;具有小毛孔的沸石,如Mor,Sapo34和Eri,很有希望,而沸石具有较大的毛孔,例如MFI,产生较重的烃。结果为CO2利用的创新催化剂设计提供了新的洞察。 (c)2021氢能出版物LLC。 elsevier有限公司出版。保留所有权利。

著录项

  • 来源
    《International journal of hydrogen energy》 |2021年第74期|36721-36730|共10页
  • 作者单位

    Ibaraki Univ Dept Mat Sci & Engn 4-12-1 Nakanarusawa Cho Hitachi Ibaraki 3168511 Japan;

    Ibaraki Univ Inst Quantum Beam Sci 4-12-1 Nakanarusawa Cho Hitachi Ibaraki 3168511 Japan;

    Ibaraki Univ Inst Quantum Beam Sci 4-12-1 Nakanarusawa Cho Hitachi Ibaraki 3168511 Japan;

    Univ Tokyo Inst Engn Innovat Bunkyo Ku Yayoi 2-11-16 Tokyo 1138656 Japan;

    Univ Tokyo Inst Engn Innovat Bunkyo Ku Yayoi 2-11-16 Tokyo 1138656 Japan|Univ Tokyo Dept Chem Syst Engn Bunkyo Ku 7-3-1 Hongo Tokyo 1138656 Japan;

    Ibaraki Univ Dept Mat Sci & Engn 4-12-1 Nakanarusawa Cho Hitachi Ibaraki 3168511 Japan;

    Ibaraki Univ Dept Mat Sci & Engn 4-12-1 Nakanarusawa Cho Hitachi Ibaraki 3168511 Japan;

    Univ Tokyo Dept Chem Syst Engn Bunkyo Ku 7-3-1 Hongo Tokyo 1138656 Japan;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Methanol; Olefin; Zeolite; Carbon dioxide; Hydrogenation;

    机译:甲醇;烯烃;沸石;二氧化碳;氢化;

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