Deep dive into the underlying cause of the carbon loss and the associated chemical processes in fatty acid hydrodeoxygenation over Ni@Hβ catalyst

IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Fuel Processing Technology Pub Date : 2024-02-12 DOI:10.1016/j.fuproc.2024.108062
Chaojie Zhu, Wenqian Fu, Yuan Zhang, Lei Zhang, Congwei Meng, Changjun Liu, Tiandi Tang
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Abstract

Identification of the underlying cause of carbon loss in fatty acid hydrodeoxygenation (HDO) on the acidic catalyst is very important to understand the reaction mechanism and design high efficiency catalyst for biomass conversion. Herein, HDO reactions of palmitic acid catalyzed by Ni supported on mesoporous Beta (HBeta-M) zeolites with different acidities were investigated. It was found that a significant carbon loss (47.5%) occurred during the entire reaction process on Ni/HBeta-M catalyst with high acid density. This is because the hexadecyl ether intermediate was formed and trapped in the porous structure of the catalyst and interacted with strong acidic sites. On the Ni/HBeta-M-0.5 catalyst with medium acid density, carbon loss occurred in the initial reaction stage because hexadecanol was trapped in the porous catalyst. Investigations further demonstrated that the hexadecyl ether intermediate can also be converted to hexadecanol and hexadecane via hydrogenolysis on Brønsted acid and Ni sites.

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深入探究 Ni@Hβ 催化剂上脂肪酸加氢脱氧过程中碳损失的根本原因及相关化学过程
查明酸性催化剂上脂肪酸加氢脱氧(HDO)过程中碳损失的根本原因对于了解反应机理和设计生物质转化的高效催化剂非常重要。在此,研究了不同酸度的介孔 Beta(HBeta-M)沸石上支撑的镍催化棕榈酸的 HDO 反应。研究发现,在高酸度的 Ni/HBeta-M 催化剂上,整个反应过程中会出现大量的碳损失(47.5%)。这是因为十六烷基醚中间体在催化剂的多孔结构中形成并被截留,并与强酸性位点相互作用。在中等酸密度的 Ni/HBeta-M-0.5 催化剂上,由于十六烷醇被截留在多孔催化剂中,因此在反应初期会出现碳损失。研究进一步证明,十六烷基醚中间体也可通过布氏酸和镍位点上的氢解作用转化为十六醇和十六烷。
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来源期刊
Fuel Processing Technology
Fuel Processing Technology 工程技术-工程:化工
CiteScore
13.20
自引率
9.30%
发文量
398
审稿时长
26 days
期刊介绍: Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.
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