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通过均匀互连的ZSM-5@AlSBA-15复合材料上的串联催化将大分子烃深度裂解为轻质产品

Deep Cracking of Bulky Hydrocarbons into Light Products via Tandem Catalysis over Uniform Interconnected ZSM-5@AlSBA-15 Composites.

作者信息

Zhang Yali, Wang Jiaren, Xie Xianglin, Wang Xiaoning, Wu Winston Duo, Chen Xiao Dong, Wu Zhangxiong

机构信息

Particle Engineering Laboratory, School of Chemical and Environmental Engineering, and Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry Chemical Engineering and Materials Science, Soochow University, Suzhou, Jiangsu, 215123, P. R. China.

出版信息

Small. 2024 Jun;20(26):e2309114. doi: 10.1002/smll.202309114. Epub 2024 Jan 17.

Abstract

Deep cracking of bulky hydrocarbons on zeolite-containing catalysts into light products with high activity, desired selectivity, and long-term stability is demanded but challenging. Herein, the efficient deep cracking of 1,3,5-triisopropylbenzene (TIPB) on intimate ZSM-5@AlSBA-15 composites via tandem catalysis is demonstrated. The rapid aerosol-confined assembly enables the synthesis of the composites composed of a continuous AlSBA-15 matrix decorated with isolated ZSM-5 nanoparticles. The two components at various ZSM-5/AlSBA-15 mass ratios are uniformly mixed with chemically bonded pore walls, interconnected pores, and eliminated external surfaces of nanosized ZSM-5. The typical composite with a ZSM-5/AlSBA-15 mass ratio of 0.25 shows superior performance in TIPB cracking with outstanding activity (≈100% conversion) and deep cracking selectivity (mass of propylene + benzene > 60%) maintained for a long time (> 6 h) under a high TIPB flux (2 mL h), far better (several to tens of times higher) than the single-component and physically mixed catalysts and superior to literature results. The high performance is attributed to the cooperative tandem catalytic process, that is, selective and timely pre-cracking of TIPB to isopropylbenzene (IPB) in AlSBA-15 and subsequently timely diffusion and deep cracking of IPB in nanosized ZSM-5.

摘要

将大分子烃高效地在含沸石催化剂上深度裂化为轻质产物,同时具备高活性、理想的选择性和长期稳定性,这是有需求的,但具有挑战性。在此,展示了通过串联催化在紧密的ZSM-5@AlSBA-15复合材料上对1,3,5-三异丙基苯(TIPB)进行高效深度裂化。快速的气溶胶受限组装能够合成由连续的AlSBA-15基质装饰有孤立的ZSM-5纳米颗粒组成的复合材料。不同ZSM-5/AlSBA-15质量比的两种组分与化学键合的孔壁、相互连接的孔以及纳米尺寸ZSM-5的外部表面被消除后均匀混合。典型的ZSM-5/AlSBA-15质量比为0.25的复合材料在TIPB裂化中表现出优异的性能,在高TIPB通量(2 mL h)下具有出色的活性(≈100%转化率)和深度裂化选择性(丙烯+苯的质量>60%)并能长时间(>6小时)保持,比单组分和物理混合催化剂要好得多(高出几倍到几十倍)且优于文献结果。高性能归因于协同串联催化过程,即TIPB在AlSBA-15中选择性且及时地预裂化为异丙基苯(IPB),随后IPB在纳米尺寸的ZSM-5中及时扩散并深度裂化。

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