The promoting role of framework Ti(IV) in enhancing the hydrodeoxygenation performance of palmitic acid over a mesoporous TS-1 supported Ni catalyst

被引:4
作者
Zhang, Yuan [1 ]
Fu, Wenqian [1 ]
Huang, Mingyu [1 ]
Liy, Li [2 ]
Zhang, Lei [1 ]
Zhu, Chaojie [1 ]
Tang, Tiandi [1 ]
机构
[1] Changzhou Univ, Sch Petrochem Engn, Changzhou 213164, Jiangsu, Peoples R China
[2] SINOPEC Dalian Res Inst Petr & Petrochem Co Ltd, Dalian 116045, Peoples R China
基金
中国国家自然科学基金;
关键词
Mesoporous TS-1 zeolite; Ni-based catalyst; Framework Ti(IV); Palmitic acid; Hydrodeoxygenation; HETEROGENEOUS ESTERIFICATION; EFFECTIVE HIERARCHIZATION; RANGE ALKANES; SOLID ACID; ZEOLITE; OXIDATION; HYDRODESULFURIZATION; DEOXYGENATION; SITES;
D O I
10.1016/j.apcata.2024.119833
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
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页数:13
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