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One-Pass Hydrogenation of CO2 to Multibranched Isoparaffins over Bifunctional Zeolite-Based Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-11-20 , DOI: 10.1021/acscatal.0c03292 Aqsa Noreen 1 , Mingquan Li 1 , Yajie Fu 1 , Cederick Cyril Amoo 1, 2 , Jiayuan Wang 1 , Elton Maturura 1 , Ce Du 1 , Ruiqin Yang 1 , Chuang Xing 1 , Jian Sun 2
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-11-20 , DOI: 10.1021/acscatal.0c03292 Aqsa Noreen 1 , Mingquan Li 1 , Yajie Fu 1 , Cederick Cyril Amoo 1, 2 , Jiayuan Wang 1 , Elton Maturura 1 , Ce Du 1 , Ruiqin Yang 1 , Chuang Xing 1 , Jian Sun 2
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Direct hydrogenation of CO2 to high-valued fuels is a process that can be likened to the “Trapping two fishes with a single worm”. This win–win situation addresses the ever-increasing problems associated with excessive CO2 emission as well as renewable energy supply. In this contribution, a thorough study is realized on 10 MR zeolites with one-dimensional (1D) and three-dimensional (3D) structures for the direct hydrogenation of CO2 to gasoline (C5–C11), with a high fraction of multibranched isoparaffins. Emphasis is placed on identifying the factors that favor isomerization and increase the number of branches on the isomers. Zeolites SAPO-11 and ZSM-5 were configured with Na/Fe3O4 (NaFe) in single-, dual-, and various triple-bed arrangements for this investigation. A dual-bed reaction with SAPO-11 and ZSM-5 coupled individually with the NaFe catalyst showed relatively higher selectivity for low-branched isoparaffins and aromatics, respectively. In the event of combining both the zeolites with NaFe as a physical mix and triple-bed systems, isoparaffins selectivity increased with improved multibranched isomers and reduced aromatics at the same time. Among these different tactics, the triple-bed system comprising the NaFe catalyst followed sequentially with SAPO-11 and ZSM-5 maximizes the selectivity for isoparaffins with the enhanced formation of multibranched isomers. The selectivity of gasoline reached 71.7% in hydrocarbons (HCs) with a maximum of 38.2% isoparaffins possessing a RON value of 91.7 at CO2 conversion of 31.2%. Multibranched isomers accounted for 28.3% in all C5+ isoparaffins, much higher than that of the single zeolite. Purposefully, hypothetical knowledge obtained from the prior model reactions on the zeolites served as a strong foundation to support and give insight into the results from the CO2 hydrogenation reactions.
中文翻译：
双功能沸石基催化剂将CO 2单程加氢成多支链异链烷烃
将CO 2直接加氢为高价值燃料的过程可以比喻为“用一条蠕虫捕获两条鱼”。这种双赢的局面解决了与过量CO 2排放以及可再生能源供应有关的日益严重的问题。在此贡献中，对10种具有一维（1D）和三维（3D）结构的MR沸石进行了深入研究，以将CO 2直接加氢为汽油（C 5 –C 11），其中大部分多支异链烷烃。重点放在确定有利于异构化并增加异构体上支链数量的因素上。分子筛SAPO-11和ZSM-5配置有Na / Fe 3 O4（NaFe）以单床，双床和各种三床布置进行此调查。SAPO-11和ZSM-5分别与NaFe催化剂偶合的双床反应分别显示出对低支链异链烷烃和芳烃的较高选择性。如果将沸石与NaFe作为物理混合物和三重床系统组合使用，则异链烷烃的选择性会随着改进的多支链异构体和减少的芳烃而增加。在这些不同的策略中，包含NaFe催化剂的三层床系统依次跟随有SAPO-11和ZSM-5，通过增强多支链异构体的形成，最大化了对异链烷烃的选择性。汽油在碳氢化合物（HCs）中的选择性达到71.7％，最高38.2％的异链烷烃在CO处的RON值为91.7。2转化率为31.2％。在所有C 5+异链烷烃中，多支链异构体占28.3％，远高于单分子沸石。有目的地从在沸石上进行的先前模型反应中获得的假设知识为支持和深入了解CO 2氢化反应的结果奠定了坚实的基础。
更新日期：2020-12-04
中文翻译：
双功能沸石基催化剂将CO 2单程加氢成多支链异链烷烃
将CO 2直接加氢为高价值燃料的过程可以比喻为“用一条蠕虫捕获两条鱼”。这种双赢的局面解决了与过量CO 2排放以及可再生能源供应有关的日益严重的问题。在此贡献中，对10种具有一维（1D）和三维（3D）结构的MR沸石进行了深入研究，以将CO 2直接加氢为汽油（C 5 –C 11），其中大部分多支异链烷烃。重点放在确定有利于异构化并增加异构体上支链数量的因素上。分子筛SAPO-11和ZSM-5配置有Na / Fe 3 O4（NaFe）以单床，双床和各种三床布置进行此调查。SAPO-11和ZSM-5分别与NaFe催化剂偶合的双床反应分别显示出对低支链异链烷烃和芳烃的较高选择性。如果将沸石与NaFe作为物理混合物和三重床系统组合使用，则异链烷烃的选择性会随着改进的多支链异构体和减少的芳烃而增加。在这些不同的策略中，包含NaFe催化剂的三层床系统依次跟随有SAPO-11和ZSM-5，通过增强多支链异构体的形成，最大化了对异链烷烃的选择性。汽油在碳氢化合物（HCs）中的选择性达到71.7％，最高38.2％的异链烷烃在CO处的RON值为91.7。2转化率为31.2％。在所有C 5+异链烷烃中，多支链异构体占28.3％，远高于单分子沸石。有目的地从在沸石上进行的先前模型反应中获得的假设知识为支持和深入了解CO 2氢化反应的结果奠定了坚实的基础。
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