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Identification of the Encapsulation Effect of Heteropolyacid in the Si–Al Framework toward Benzene Alkylation
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-04-06 , DOI: 10.1021/acscatal.1c05895 Yuan Liu 1 , Qiaoyun Liu 1 , Kaihang Sun 2 , Shufang Zhao 3 , Young Dok Kim 3 , Yongpeng Yang 1 , Zhongyi Liu 1 , Zhikun Peng 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-04-06 , DOI: 10.1021/acscatal.1c05895 Yuan Liu 1 , Qiaoyun Liu 1 , Kaihang Sun 2 , Shufang Zhao 3 , Young Dok Kim 3 , Yongpeng Yang 1 , Zhongyi Liu 1 , Zhikun Peng 1
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Heterogenization of homogeneous catalysts is a long-term pursuit in the field of catalysis application. Traditional alkylation of arenes with olefins is usually achieved using acid catalysts in a homogeneous system, with high catalytic activity and selectivity but difficulty in catalyst separation and reusability. Herein, H3PW12O40 (HPW), an excellent homogeneous Brønsted acid catalyst, was anchored to the faujasite (FAU) cage of ultrastable Y (USY) zeolite with high dispersion (HPW@USY). 100% conversion of cyclohexene (CHE) with 99.9% yield of cyclohexylbenzene was obtained by the alkylation of benzene (C6H6) and CHE (VC6H6/VCHE= 7:1). No obvious deactivation was observed over HPW@USY after eight cycles. Our experimental and theoretical results demonstrated that W–OH exposed in HPW, encapsulated in the FAU cage, is the active site for alkylation. The excellent performance of the HPW@USY catalyst was attributed to the homogeneous chemical environment and stability of the encapsulated HPW. Benefiting from the formation and stabilization of a reaction intermediate (C6H11•) during the CHE activation, the encapsulation effect of HPW in the Si–Al framework played a significant role in the alkylation between CHE and other aromatic hydrocarbons with high yields of alkylated products. This work provides a promising heterogeneous catalyst strategy, making the alkylation efficiency of aromatics and olefins as high as that of homogeneous catalysts.
中文翻译：
Si-Al骨架中杂多酸对苯烷基化的包封作用的鉴定
均相催化剂的多相化是催化应用领域的长期追求。传统的芳烃与烯烃烷基化反应通常采用酸性催化剂在均相体系中实现，具有较高的催化活性和选择性，但催化剂分离和重复使用困难。在此，H 3 PW 12 O 40 (HPW) 是一种优异的均相布朗斯台德酸催化剂，被锚定在具有高分散性的超稳定 Y (USY) 沸石 (HPW@USY) 的八面沸石 (FAU) 笼上。通过苯(C 6 H 6 )和环己烯(CHE)( V C 6 H 6 /V )的烷基化反应得到环己烯(CHE)的100%转化率和99.9%的环己基苯收率车= 7:1)。八次循环后，HPW@USY 未观察到明显的失活。我们的实验和理论结果表明，暴露在 HPW 中、封装在 FAU 笼中的 W-OH 是烷基化的活性位点。HPW@USY 催化剂的优异性能归因于均匀的化学环境和封装的 HPW 的稳定性。受益于反应中间体 (C 6 H 11 •) 在 CHE 活化过程中，HPW 在 Si-Al 骨架中的包封作用在 CHE 与其他芳烃之间的烷基化中发挥了重要作用，烷基化产物的收率很高。这项工作提供了一种很有前景的多相催化剂策略，使芳烃和烯烃的烷基化效率与均相催化剂一样高。
更新日期：2022-04-06
中文翻译：
Si-Al骨架中杂多酸对苯烷基化的包封作用的鉴定
均相催化剂的多相化是催化应用领域的长期追求。传统的芳烃与烯烃烷基化反应通常采用酸性催化剂在均相体系中实现，具有较高的催化活性和选择性，但催化剂分离和重复使用困难。在此，H 3 PW 12 O 40 (HPW) 是一种优异的均相布朗斯台德酸催化剂，被锚定在具有高分散性的超稳定 Y (USY) 沸石 (HPW@USY) 的八面沸石 (FAU) 笼上。通过苯(C 6 H 6 )和环己烯(CHE)( V C 6 H 6 /V )的烷基化反应得到环己烯(CHE)的100%转化率和99.9%的环己基苯收率车= 7:1)。八次循环后，HPW@USY 未观察到明显的失活。我们的实验和理论结果表明，暴露在 HPW 中、封装在 FAU 笼中的 W-OH 是烷基化的活性位点。HPW@USY 催化剂的优异性能归因于均匀的化学环境和封装的 HPW 的稳定性。受益于反应中间体 (C 6 H 11 •) 在 CHE 活化过程中，HPW 在 Si-Al 骨架中的包封作用在 CHE 与其他芳烃之间的烷基化中发挥了重要作用，烷基化产物的收率很高。这项工作提供了一种很有前景的多相催化剂策略，使芳烃和烯烃的烷基化效率与均相催化剂一样高。
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