框架 Ti(IV) 在介孔 TS-1 支持的 Ni 催化剂上对提高棕榈酸加氢脱氧性能的促进作用

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-06-05 DOI:10.1016/j.apcata.2024.119833
Yuan Zhang , Wenqian Fu , Mingyu Huang , Li Liu , Lei Zhang , Chaojie Zhu , Tiandi Tang
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引用次数: 0

摘要

开发高效的镍基加氢脱氧催化剂对于生产可再生生物柴油至关重要。在本文中,介孔 TS-1 沸石支撑的 Ni 催化剂(Ni/TS-1-M)表现出优异的加氢脱氧(HDO)活性,脱氧烃的产率达到 100%(97.3% 的十五烷对 2.7% 的十六烷),优于其他催化剂,如介孔 ZSM-5 上的 Ni(Ni/ZSM-5-M)、介孔硅胶石-1(Ni/硅胶石-1-M)和 TiO2(Ni/TiO2)。TiO4和TiO6形式的Ti(IV)原子可将其电子传递给附近的金属Ni,导致金属Ni的电子密度增加,从而提高了氢化活性,促进了十六烷醛的C-C键裂解生成十五烷。此外,在 Ni/TS-1-M 催化剂上金属 Ni 和 Ti(IV) 的协同作用下,框架 Ti(IV) 物种加速了生成棕榈酸棕榈酯的酯化过程,而棕榈酸棕榈酯很容易氢解为十六烷醇的主要中间体。生成的十六醇主要经过连续脱氢/脱羰基过程转化为十五烷。
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The promoting role of framework Ti(IV) in enhancing the hydrodeoxygenation performance of palmitic acid over a mesoporous TS-1 supported Ni catalyst

Developing a highly efficient Ni-based hydrodeoxygenation catalyst is crucial for the production of renewable biodiesel. Herein, a mesoporous TS-1 zeolite supported Ni catalyst (Ni/TS-1-M) exhibited exceptional hydrodeoxygenation (HDO) activity and achieved 100 % yield of deoxygenated hydrocarbons (97.3 % pentadecane vs 2.7 % hexadecane), outperforming other catalysts such as Ni on mesoporous ZSM-5 (Ni/ZSM-5-M), mesoporous Silicalite-1 (Ni/Silicalite-1-M) and TiO2 (Ni/TiO2). The Ti(IV) atoms in the form of TiO4 and TiO6 can transfer its electron to nearby metal Ni, leading to the increase in electron density of metal Ni, which enhanced the hydrogenation activity and facilitated the C–C bond cleavage of the hexadecanal to produce pentadecane. Furthermore, the framework Ti(IV) species accelerated the esterification process to generate palmityl palmitate, which was easily hydrogenolyzed to the main intermediate of hexadecanol under the synergistic effect of metal Ni and Ti(IV) on Ni/TS-1-M catalyst. The formed hexadecanol mainly underwent successive dehydrogenation/decarbonylation process to transform into pentadecane.

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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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