Oligomerization of ethylene to linear α-olefins catalyzed by Versailles/Santa Barbara-1 with LiAlH4

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-02-05 Epub Date: 2024-12-19 DOI:10.1016/j.apcata.2024.120085
Cong Wang, Gang Li, Zheng Huang, Anfeng Peng
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Abstract

Alkyl-aluminum, which is sensitive to air, has been a major obstacle to the development of ethylene oligomerization. Herein, LiAlH4 is used as an effective alkyl-aluminum substitute. The performance of LiAlH4 itself in the reaction is investigated, proving that it possesses moderate activity. Further addition of Versailles/Santa Barbara-1 (VSB-1) catalysts with different morphologies can effectively improve the reaction, in which VSB-1/LiAlH4 presents the activity of 32.1 ggLiAlH4−1·h−1 (154.1 ggVSB-1−1‧h−1) and the selectivity of 1-butene, 1-hexene and 1-octene in all products could reach 51.4 %, 18.9 % and 7.9 %, respectively. The co-catalytic system is stable and the VSB-1 catalyst therein can be effectively reused at least three times under the suitable treatment conditions. In addition, the product analysis of the co-catalyzed system reveals that the addition of VSB-1 catalyst tended to produce 1-butene, 1-hexene and 1-octene at 20 bar. Based on above result, a possible reaction mechanism is proposed.
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在Versailles/Santa Barbara-1催化下,LiAlH4催化乙烯低聚生成线性α-烯烃
烷基铝对空气敏感,一直是乙烯低聚发展的主要障碍。本文采用LiAlH4作为烷基铝的有效替代品。研究了LiAlH4本身在反应中的表现,证明其具有中等活性。进一步加入不同形态的Versailles/Santa Barbara-1 (vbs -1)催化剂,可以有效地改善反应,其中vbs -1/LiAlH4的活性为32.1 g·gLiAlH4−1·h−1(154.1 g·gvbs -1−1·h−1),1-丁烯、1-己烯和1-辛烯的选择性分别达到51.4% %、18.9 %和7.9 %。该共催化体系稳定,其中的VSB-1催化剂在合适的处理条件下可有效重复使用至少三次。此外,共催化体系的产物分析表明,VSB-1催化剂的加入倾向于在20 bar下生成1-丁烯、1-己烯和1-辛烯。在此基础上,提出了一种可能的反应机理。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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