In situ modification of heavy oil catalyzed by nanosized metal-organic framework at mild temperature and its mechanism

原位 催化作用 机制(生物学) 金属 材料科学 化学工程 纳米技术 化学 冶金 有机化学 工程类 物理 量子力学
作者
Li Wang,Jixiang Guo,Ruiying Xiong,Chen-Hao Gao,Xiaojun Zhang,Dan Luo
出处
期刊:Chinese Journal of Chemical Engineering [Elsevier BV]
卷期号:67: 166-173 被引量:1
标识
DOI:10.1016/j.cjche.2023.11.023
摘要

Two catalysts, nano-sized cobalt-metal-organic framework (Co-MOF) and nickel (Ni)-MOF, were successfully prepared by the modification method. Tetralin (C10H12) was used as the hydrogen donor for the catalytic cracking and hydrogenation modification study of the dehydrated crude oil from the Shengli Oilfield. The optimal reaction conditions were determined through orthogonal experiments, and the components of the crude oil and modified oil samples were analyzed. The results revealed that the nano-MOF catalysts were successfully prepared and exhibited high catalytic activity. They could catalyze the cracking of large molecules in heavy oil at mild temperatures (<300 °C), leading to the decomposition of the hydrogen donor. When the mass fraction of the catalyst was 0.2%, the mass fraction of the hydrogen donor was 1%, and the reaction temperature was 280 °C, the Ni-MOF showed the best catalytic viscosity reduction effect. It could reduce the viscosity of heavy oil at 50 °C from 15761.9 mPa·s to 1266.2 mPa·s, with a viscosity reduction rate of 91.97%. The modification effect of Co-MOF was the next best, which could reduce the viscosity of heavy oil to 2500.1 mPa·s with a viscosity reduction rate of 84.14%. Molecular dynamics simulations revealed a strong interaction force between the MOF surface and asphaltene molecules. In the process of heavy-oil catalytic hydrogenation, the nano-MOF catalyst exhibited high catalytic activity. On the one hand, the empty d orbitals outside the metal atoms in the catalyst could polarize the carbon atoms in the organic matter, accelerating the breaking of long chains. On the other hand, the metal atoms in the catalyst could bond with the carbon σ bonds, breaking the carbon–carbon bonds. This disrupted the structure of the recombined components in the crude oil, irreversibly reducing the viscosity of the heavy oil and improving its fluidity.
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