路易斯酸度对基质的调节及其在轻烃催化裂解中的性能

Q3 Energy 燃料化学学报 Pub Date : 2024-02-01 DOI:10.1016/S1872-5813(23)60383-4
Rui FENG , Zhou FANG , Peng ZHOU , Tianbo LI , Xiaoyan HU , Xinlong YAN , Zhongdong ZHANG
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引用次数: 0

摘要

在石脑油催化裂化过程中,沸石与基质的合理匹配是提高轻烯烃产率的最有效策略之一。然而,基质表面路易斯酸度对裂解反应的影响仍不明确。因此,本研究采用硼锌共改性γ-Al2O3 和锡改性介孔二氧化硅 KIT-6(其表面路易斯酸度可调)来评估正庚烷和 1-己烯裂解为轻质烯烃的反应活性,其中基质单独使用或与 ZSM-5 沸石以不同的填料模式耦合使用。通过 XRD、TEM、N2 物理吸收-解吸和 NH3-TPD,研究了改性剂对 γ-Al2O3 和 KIT-6 的质地特性和表面酸度的影响。结果表明,B 的掺杂降低了 γ-Al2O3 的路易斯酸度(包括量和酸强度),而 Zn 的掺杂则增加了路易斯酸度。此外,有序介孔 KIT-6 的路易斯酸度随着 Sn 掺杂量的增加而增加。对于纯基质,正庚烷和 1-hexene 转化率的上升与 B 和 Zn 共修饰的 γ-Al2O3 和 xSn/KIT-6 的路易斯酸度增加以及活化能降低是一致的。与此相反,当与 ZSM-5 沸石耦合时,基质和沸石的双床方式实现了最高的转化率,并且转化率随着基质路易斯酸度的增加而增加。然而,过高的路易斯酸度会加快氢转移速度,同时降低轻烯烃的选择性。
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Regulation of the Lewis acidity on matrix and their performance in the catalytic cracking of light hydrocarbons

The reasonable matching of zeolite and matrix is one of the most effective strategies to increase the yield of light olefins in naphtha catalytic cracking. However, the influence of the surface Lewis acidity within the matrix on the cracking reactions has remained ambiguous. Therefore, in present study, boron and zinc co-modified γ-Al2O3 and tin modified mesoporous silica KIT-6 with tuned surface Lewis acidity were applied to evaluate the cracking reactivity of n-heptane and 1-hexene to light olefins, in which the matrix was used alone and coupled with ZSM-5 zeolite in different packed modes. The effects of the modifiers on the textural properties and surface acidity of γ-Al2O3 and KIT-6 were investigated by XRD, TEM, N2 physical absorption-desorption, and NH3-TPD. The results showed that B doping reduced the Lewis acidity (both in the amount and acid strength) of γ-Al2O3, while the incorporation of Zn doping led to increased Lewis acidity. In addition, the Lewis acidity of ordered mesoporous KIT-6 increased as Sn doping rose. While for pure matrix, the ascend in conversions of n-heptane and 1-hexene was consistent with the increased Lewis acidity of the B and Zn co-modified γ-Al2O3 and xSn/KIT-6 rose, along with decreased activation energy. In contrast, when coupled with ZSM-5 zeolite, the highest conversion was achieved in the dual-bed manner of matrix and zeolite, and the conversion increased concomitantly with the increase in the Lewis acidity of the matrix. However, excessive Lewis acidity can accelerate the hydrogen transfer rate while diminishing the selectivity of light olefins.

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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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