Huanglan Xue, Yu Huang, Yi Li, Yongfan Zhang, Wei Lin
{"title":"Computational screening of single-atom catalysts supported on triazine-based graphite carbon nitride for 1,2-dichloroethane dechlorination.","authors":"Huanglan Xue, Yu Huang, Yi Li, Yongfan Zhang, Wei Lin","doi":"10.1063/5.0288228","DOIUrl":null,"url":null,"abstract":"<p><p>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.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1000,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1063/5.0288228","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
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.
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.