三嗪基石墨氮化碳负载单原子1,2-二氯乙烷脱氯催化剂的计算筛选

IF 3.1 2区 化学 Q3 CHEMISTRY, PHYSICAL
Huanglan Xue, Yu Huang, Yi Li, Yongfan Zhang, Wei Lin
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引用次数: 0

摘要

在本研究中,我们通过密度泛函理论计算系统地研究了八种过渡金属原子负载三嗪基石墨氮化碳(TM@TGCN)催化1,2-二氯乙烷(1,2- dce)脱氯反应(DCEDR)的性能。通过五步筛选法,最终确定了分别适用于生成氯乙烯(CH2CHCl)、乙烯(CH2CH2)和乙烷(CH3CH3)的合适催化剂。Fe@TGCN还原1,2- dce为CH3CH3的极限电位较低,分别为-0.47 V(间扭式c2h4cl2)和-0.50 V(反式c2h4cl2)。活性机理表明Fe@TGCN位于火山图的顶点,证实其与反应物的相互作用强度处于最优平衡状态。此外,我们还进一步考察了羟基改性对DCEDR选择性的影响。结果表明,羟基改性通过位阻效应和电子离域显著减弱了中间产物(如*CH2CH2Cl)的吸附强度,降低了CH2CH2的解吸能,增强了其选择性。本研究为DCEDR电催化剂的合理设计提供了理论指导,揭示了配体修饰策略在调节反应途径中的关键作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Computational screening of single-atom catalysts supported on triazine-based graphite carbon nitride for 1,2-dichloroethane dechlorination.

In this study, we systematically investigated the performance of eight transition metal atom-loaded triazine-based graphitic carbon nitride (TM@TGCN) for the catalysis of 1,2-dichloroethane (1,2-DCE) dechlorination reaction (DCEDR) by density functional theory calculations. Through the five-step screening method, the suitable catalysts, respectively, applicable to the generation of vinyl chloride (CH2CHCl), ethylene (CH2CH2), and ethane (CH3CH3) were finally determined. The limiting potential of Fe@TGCN for reducing 1,2-DCE to CH3CH3 is lower, at -0.47 V (gauche-C2H4Cl2) and -0.50 V (trans-C2H4Cl2), respectively. The activity mechanism indicates that Fe@TGCN is at the vertex of the volcano plot, confirming that the intensity of its interaction with the reactants is in optimal equilibrium. In addition, we further examined the influence of hydroxyl modification on the selectivity of DCEDR. The results show that hydroxyl modification significantly weakens the adsorption strength of intermediates (such as *CH2CH2Cl) through a steric hindrance effect and electron delocalization, as well as reduces the desorption energy of CH2CH2 and enhances its selectivity. This study provides theoretical guidance for the rational design of DCEDR electrocatalysts and reveals the key role of ligand modification strategies in regulating the reaction pathway.

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来源期刊
Journal of Chemical Physics
Journal of Chemical Physics 物理-物理:原子、分子和化学物理
CiteScore
7.40
自引率
15.90%
发文量
1615
审稿时长
2 months
期刊介绍: The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance. Topical coverage includes: Theoretical Methods and Algorithms Advanced Experimental Techniques Atoms, Molecules, and Clusters Liquids, Glasses, and Crystals Surfaces, Interfaces, and Materials Polymers and Soft Matter Biological Molecules and Networks.
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