C9石油树脂在多孔γ-Al2O3中的扩散特性：分子动力学研究

IF 3.9 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Langmuir Pub Date : 2025-03-16 DOI:10.1021/acs.langmuir.5c00353

Caijie Wang, Feng Zhang, Zhibing Zhang

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引用次数: 0

摘要

C9石油树脂加氢反应是典型的大分子非均相催化反应，能显著提高材料的热稳定性和相容性。这些大分子在催化剂孔内的扩散显著影响着孔内的传质和整个加氢过程。然而，由于实验的限制，孔隙中反应物的扩散率仍然难以确定，这影响了催化反应过程的精确设计和操作。通过考虑原子电荷，建立了一个更真实的γ-Al2O3模型，并利用INTERFACE力场描述了客体分子与γ-Al2O3之间更精确的相互作用。通过计算可达表面积、总孔隙体积、羟基密度、广角x射线衍射图和苯吸附等指标对模型进行表征。对计算结果进行了验证，并与相应的实验室数据进行了比较。通过分子动力学模拟进一步评价了C9石油树脂在生成的γ-Al2O3中的扩散行为。考察了温度、C9石油树脂的动力学直径、γ-Al2O3的孔径和孔窗尺寸对扩散性能的影响。研究发现，温度升高可以加速分子扩散，较大的分子对温度变化更敏感。在给定的γ-Al2O3孔隙结构下，C9石油树脂的扩散系数与动力学直径呈线性关系。在一定的动力学直径下，C9石油树脂的扩散系数与孔径呈抛物线关系，而孔窗大小对C9石油树脂的扩散有重要影响。这些结果为制备可行的C9石油树脂加氢多孔γ-Al2O3催化剂提供了优化的操作条件和有价值的指导。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Diffusion Properties of C9 Petroleum Resin in Porous γ-Al2O3: A Molecular Dynamics Study

查看原文本刊更多论文

Diffusion Properties of C9 Petroleum Resin in Porous γ-Al2O3: A Molecular Dynamics Study

C9 petroleum resin hydrogenation is a classic macromolecular heterogeneous catalyzed reaction that can markedly improve the material’s thermal stability and compatibility. The diffusion of these macromolecules within the catalyst pores significantly influences the mass transfer there and the overall hydrogenation process. However, due to experimental limitations, the diffusivity of reactants in the pores remains challenging to determine, which affects the accurate design and operation of the catalytic reaction process. A more realistic model of γ-Al₂O₃ was developed by incorporating atomic charge considerations, and a more precise interaction between the guest molecule and γ-Al₂O₃ was described using the INTERFACE force field. The model was characterized by calculating the accessible surface area, total pore volume, hydroxyl group density, wide-angle X-ray diffraction patterns, and benzene adsorption. The calculated results were validated and compared with the corresponding laboratory data. Molecular dynamics simulations were further employed to evaluate the diffusion behavior of C9 petroleum resin within the generated γ-Al₂O₃. The effects of temperature, the kinetic diameter of C9 petroleum resin, pore size, and pore window size of γ-Al₂O₃ on diffusion performance were examined. It was found that an increase in temperature can accelerate molecular diffusion, with larger molecules being more sensitive to temperature variations. A linear relationship between the diffusion coefficient and the kinetic diameter of C9 petroleum resin was observed for a given γ-Al₂O₃ pore structure. Additionally, the diffusion coefficient exhibited a parabolic dependence on pore size at a constant kinetic diameter, while the pore window size had a crucial influence on the diffusion of C9 petroleum resin. These results provide optimized operating conditions and valuable guidance for the preparation of feasible porous γ-Al₂O₃ catalysts for C9 petroleum resin hydrogenation.

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来源期刊

Langmuir 化学-材料科学：综合

CiteScore

6.50

自引率

10.30%

发文量

1464

审稿时长

2.1 months

期刊介绍： Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).