Effect of Al Location and Ga Species in ZSM-5 on Adsorption of Soluble Coke

IF 2.9 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Journal of Computational Chemistry Pub Date : 2026-09-23 DOI:10.1002/jcc.70515

Jinping Liu, Hongyan Liu, Lixia Ling, Caiping Ma, Riguang Zhang, Yang Zhang, Maohong Fan, Baojun Wang

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引用次数: 0

Abstract

During the methanol-to-hydrocarbons process catalyzed by H-ZSM-5, coke deposition occurs and can severely hinder the reaction. The effect of Al location and Ga species in ZSM-5 on the adsorption of soluble coke was investigated using density functional theory calculations with the ONIOM method. The results show that soluble coke is adsorbed more stably when Al is situated at straight channels and channel intersections than that in the sinusoidal channel. For Ga species, Ga(OH)²⁺, GaO⁺ and GaH²⁺ are found to readily adsorb soluble coke compared with GaH₂⁺, GaH(OH)⁺, and Ga⁺. Further analysis reveals that the acid strength of Ga species does not exhibit a linear correlation with the adsorption energy of soluble coke. Apart from pyrene that fails to be stably adsorbed, the charge variation of Ga species shows an inverted-volcano-shaped correlation with the adsorption energies of aromatics. Our work provides theoretical references and data support for the design of anti-coking zeolite catalysts and the precise regulation of active sites.

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ZSM-5中Al位置和Ga种类对可溶性焦炭吸附的影响

在H-ZSM-5催化甲醇制烃过程中，会产生焦炭沉积，严重阻碍反应的进行。采用密度泛函理论计算和onom方法研究了ZSM-5中Al位置和Ga种类对可溶性焦炭吸附性能的影响。结果表明，Al在直线通道和通道交叉处的吸附比在正弦通道中的吸附更稳定。与GaH2+、GaH(OH)+和Ga+相比，Ga(OH)2+、GaO+和GaH2+更容易吸附可溶性焦炭。进一步分析表明，Ga的酸强度与可溶性焦炭的吸附能不呈线性相关关系。除芘不能被稳定吸附外，Ga的电荷变化与芳烃的吸附能呈倒火山型相关。本研究为抗焦化沸石催化剂的设计和活性位点的精确调控提供了理论参考和数据支持。

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来源期刊

Journal of Computational Chemistry 化学-化学综合

CiteScore

6.60

自引率

3.30%

发文量

247

审稿时长

1.7 months

期刊介绍： This distinguished journal publishes articles concerned with all aspects of computational chemistry: analytical, biological, inorganic, organic, physical, and materials. The Journal of Computational Chemistry presents original research, contemporary developments in theory and methodology, and state-of-the-art applications. Computational areas that are featured in the journal include ab initio and semiempirical quantum mechanics, density functional theory, molecular mechanics, molecular dynamics, statistical mechanics, cheminformatics, biomolecular structure prediction, molecular design, and bioinformatics.