Rh- 包封 ZSM-5 催化剂上的金属辅助正己烷低温裂解

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-05-28 DOI:10.1016/j.micromeso.2024.113199
Hiroyasu Fujitsuka , Mai Yamaji , Rikako Nakatani , Misaki Endoh , Teruoki Tago
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引用次数: 0

摘要

石脑油裂解是生产乙烯、丙烯和丁烯等轻烯烃的最常见工艺。该工艺能耗巨大,因此降低能耗和操作温度是一个亟待解决的问题。为了降低石脑油裂解的反应温度,我们重点研究了金属辅助裂解反应,即在金属催化剂上首先将石蜡脱氢为相应的烯烃,然后将生成的烯烃分解为轻质烯烃。为了有效实现金属辅助裂解,我们认为金属封装沸石催化剂非常有用。在金属封装沸石催化剂中,脱氢反应在沸石颗粒内部进行,脱氢中间产物可以频繁进入固酸位点。本研究将 Rh 纳米粒子包封 ZSM-5 催化剂(Rh@ZSM-5)用于正己烷的金属辅助裂解。由于Rh@ZSM-5的金属封装结构以及金属和固酸位点之间的紧密性,它在450 °C以下的正己烷裂解过程中表现出明显的高活性。此外,还研究了反应条件、反应温度、金属和固酸位点的数量以及接触时间对 Rh@ZSM-5 催化剂上金属辅助正己烷裂解的影响。在 Rh@ZSM-5 上转化正己烷时,Rh 的负载量为 0.3 wt%,Si/Al 比为 100,温度为 450 °C,反应时间为 0.5 h,W/F 为 2 h,轻烯烃产量最高,达到 38.6 碳摩尔%。
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Metal-assisted low-temperature cracking of n-hexane over Rh-encapsulated ZSM-5 catalysts

Naphtha cracking is the most common process for producing light olefins such as ethylene, propylene, and butene. This process consumes enormous amounts of energy, so decreasing the energy consumption and operating temperature is an urgent issue. To decrease the reaction temperature for naphtha cracking, we focused on the metal-assisted cracking reaction, in which paraffin is first dehydrogenated into the corresponding olefin on a metal catalyst, and the produced olefin is then decomposed into light olefins. To effectively realize metal-assisted cracking, we considered metal-encapsulated zeolite catalysts to be useful. In metal-encapsulated zeolite catalysts, the dehydrogenation reaction proceeds inside the zeolite particles, and the dehydrogenated intermediates can access the solid-acid sites frequently. In this study, Rh nanoparticle encapsulated ZSM-5 catalysts (Rh@ZSM-5) were employed for the metal-assisted cracking of n-hexane. Rh@ZSM-5 exhibited significantly high activity for n-hexane cracking below 450 °C owing to the metal encapsulation structure and close proximity between the metal and solid-acid sites. Furthermore, the effects of reaction conditions, reaction temperature, amounts of metal and solid-acid sites, and contact time on metal-assisted n-hexane cracking over the Rh@ZSM-5 catalysts were investigated. The highest light-olefin yield of 38.6 carbon mol% was achieved by the conversion of n-hexane over Rh@ZSM-5 using 0.3 wt% Rh loading, an Si/Al ratio of 100, temperature of 450 °C, reaction time of 0.5 h, and W/F of 2 h.

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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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