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Effects of nanosheet catalysts on synthesis of aromatics and light hydrocarbons from acetylene
Catalysis Today ( IF 5.3 ) Pub Date : 2020-01-07 , DOI: 10.1016/j.cattod.2020.01.004
Taehee Lee , Yeongkwang Bae , Jonghyun Jeon , Juchan Kim , Jungkyu Choi , Kyoung-Su Ha

A nanosheet zeolite ITQ-2 formed by delamination of MCM-22 zeolite precursor was used and tested as a catalyst for the aromatization of acetylene. Along with MCM-22 (calcined form of MCM-22 zeolite precursor) zeolites, the resulting materials were successfully prepared and characterized in terms of pore structure and surface property. The performance of aromatization of ITQ-2 zeolites was comparable to that of MCM-22 zeolites. Due to the isolated and thin-layer structure, ITQ-2 zeolites had a significant fraction of external active sites. This feature seemed to result in relatively higher amount of C3–C8 aliphatic compounds rather than the C6–C8 aromatic compounds because of the shortened residence and, thus, reaction time. We first found that the cumulative C3–C8 aliphatic products in the case of ITQ-2 zeolites increased with the amounts of external surface area, while no clear relation was observed for the case of MCM-22 zeolites. Second, the initial selectivity towards aromatics was found to clearly show a linear relation with the concentration of Brønsted acid sites regardless of the used catalyst. In addition, the nanosheet ITQ-2 zeolites showed a much slower deactivation unlike the traditional microporous MCM-22 zeolites. Finally, to investigate the difference in the catalytic performance, we rebuilt the reaction pathways from acetylene to the aromatics and aliphatics.



中文翻译:

纳米片催化剂对乙炔合成芳烃和轻烃的影响

使用通过将MCM-22沸石前体分层而形成的纳米片状沸石ITQ-2,并将其测试为乙炔芳构化的催化剂。连同MCM-22(MCM-22沸石前体的煅烧形式)沸石一起,成功制备了所得材料,并根据孔结构和表面性质对其进行了表征。ITQ-2沸石的芳构化性能与MCM-22沸石相当。由于隔离的薄层结构,ITQ-2沸石具有很大一部分的外部活性位。由于缩短了停留时间,因此缩短了反应时间,该功能似乎导致相对于C6-C8芳香族化合物而言,C3-C8脂肪族化合物的含量相对较高。我们首先发现,在ITQ-2沸石的情况下,累积的C3-C8脂肪族产物随外表面积的增加而增加,而对于MCM-22沸石,则没有明显的关系。第二,发现对芳族化合物的初始选择性清楚地显示出与布朗斯台德酸位点的浓度呈线性关系,而与所使用的催化剂无关。此外,与传统的微孔MCM-22沸石不同,ITQ-2纳米片沸石的失活速度要慢得多。最后,为了研究催化性能的差异,我们重建了从乙炔到芳族化合物和脂族化合物的反应途径。不论使用何种催化剂,发现对芳烃的初始选择性均与布朗斯台德酸位点的浓度呈线性关系。此外,与传统的微孔MCM-22沸石不同,ITQ-2纳米片沸石的失活速度要慢得多。最后,为了研究催化性能的差异,我们重建了从乙炔到芳族化合物和脂族化合物的反应途径。无论使用何种催化剂,发现对芳烃的初始选择性均与布朗斯台德酸位点的浓度呈线性关系。此外,与传统的微孔MCM-22沸石不同,ITQ-2纳米片沸石的失活速度要慢得多。最后,为了研究催化性能的差异,我们重建了从乙炔到芳族化合物和脂族化合物的反应途径。

更新日期:2020-01-07
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