{"title":"Evaluating the Dehydrogenation Performance of Cyclohexane on Pt-Skin AgPt3(111) and Ag3Pt(111) Surface Slabs: A Density Functional Theory Approach","authors":"Desalegn Nigatu Gemechu, Kingsley Onyebuchi Obodo, Ahmed Mustefa Mohammed, Yedilfana Setarge Mekonnen","doi":"10.1021/acs.jpcc.4c05825","DOIUrl":null,"url":null,"abstract":"The development of highly effective dehydrogenation catalysts presents significant potential for storing hydrogen solutions with favorable economic advantages. In this study, we examined the dehydrogenation of cyclohexane on Pt-skin AgPt<sub>3</sub>(111) and Ag<sub>3</sub>Pt(111) surfaces in comparison with that on a Pt(111) pristine surface by applying density functional theory. We assessed the performance of various exchange–correlation functionals (PBE, BEEF-vdW, optPBE-vdW, and PBE-D3) in predicting the adsorption energy of cyclohexane on Pt–AgPt<sub>3</sub>(111), Pt–Ag<sub>3</sub>Pt(111), and Pt(111) surfaces and compared them to the experimental data. Through systematic calculations, we analyzed the electronic and structural properties of catalysts, adsorption energies of cyclohexane and intermediate molecules on various Ag–Pt alloy surfaces, surface charge distribution, dehydrogenation processes, and the effect of Ag concentration on its activity. The findings indicate that an increase in the Ag content leads to a closer shift of the d-band center of the Pt atom toward the Fermi level, moving from −2.31 to −1.81 eV. This shift increases surface charge accumulation. This gradual accumulation enhances the adsorption of cyclohexane. Notably, the dehydrogenation of cyclohexane on Pt-skin Ag<sub>3</sub>Pt exhibited a lower reaction energy, with a value of 1.31 eV compared to the pristine Pt(111) catalyst. This study revealed that the Pt-skin Ag<sub>3</sub>Pt(111) catalyst exhibits enhanced performance for the dehydrogenation of cyclohexane, which should stimulate additional experimental studies.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"82 1","pages":""},"PeriodicalIF":3.3000,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpcc.4c05825","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The development of highly effective dehydrogenation catalysts presents significant potential for storing hydrogen solutions with favorable economic advantages. In this study, we examined the dehydrogenation of cyclohexane on Pt-skin AgPt3(111) and Ag3Pt(111) surfaces in comparison with that on a Pt(111) pristine surface by applying density functional theory. We assessed the performance of various exchange–correlation functionals (PBE, BEEF-vdW, optPBE-vdW, and PBE-D3) in predicting the adsorption energy of cyclohexane on Pt–AgPt3(111), Pt–Ag3Pt(111), and Pt(111) surfaces and compared them to the experimental data. Through systematic calculations, we analyzed the electronic and structural properties of catalysts, adsorption energies of cyclohexane and intermediate molecules on various Ag–Pt alloy surfaces, surface charge distribution, dehydrogenation processes, and the effect of Ag concentration on its activity. The findings indicate that an increase in the Ag content leads to a closer shift of the d-band center of the Pt atom toward the Fermi level, moving from −2.31 to −1.81 eV. This shift increases surface charge accumulation. This gradual accumulation enhances the adsorption of cyclohexane. Notably, the dehydrogenation of cyclohexane on Pt-skin Ag3Pt exhibited a lower reaction energy, with a value of 1.31 eV compared to the pristine Pt(111) catalyst. This study revealed that the Pt-skin Ag3Pt(111) catalyst exhibits enhanced performance for the dehydrogenation of cyclohexane, which should stimulate additional experimental studies.
期刊介绍:
The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.