DICP OpenIR
Ethylene glycol reforming on Pt(111): first-principles microkinetic modeling in vapor and aqueous phases
Faheem, Muhammad1,2; Saleheen, Mohammad1; Lu, Jianmin1,3; Heyden, Andreas1
Source PublicationCatalysis Science & Technology
2016
DOI10.1039/c6cy02111e
Volume6Issue:23Pages:8242-8256
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS KeywordSUPPORTED PLATINUM CATALYSTS ; FINDING SADDLE-POINTS ; RATE-DETERMINING STEP ; ZETA VALENCE QUALITY ; BASIS-SETS ; METHANOL DECOMPOSITION ; TRANSITION-METALS ; OXYGENATED HYDROCARBONS ; RENEWABLE HYDROGEN ; ENERGY
AbstractFirst-principles, periodic density functional theory (DFT) calculations and mean-field microkinetic modeling have been used to investigate the decomposition of ethylene glycol for hydrogen production on Pt(111) in vapor and aqueous phases. All dehydrogenated species derived from ethylene glycol (C2HxO2, x = 0-6) and methanol (CHyO, y = 0-4), and all elementary C-C, C-H, and O-H bond breaking steps are included in the microkinetic model. Reaction path analysis in vapor phase indicates that both initial C-H and O-H dehydrogenation steps are kinetically relevant at all temperatures (470-530 K). Initial O-H bond cleavage is reversible at low temperatures but accounts for an increasingly dominant fraction of the total reaction flux at higher temperatures. C-C bond scission is observed only after significant dehydrogenation (x = 3) and is more likely to happen in surface intermediates where one of the cleavage products is CO. The process is highly selective to the production of H-2 compared to methanol. For aqueous-phase model development, free energies of solvation were computed for all surface intermediates and transition states using a continuum solvation approach. Our aqueous-phase microkinetic model predicts a 0.4 eV lower apparent activation energy and an order of magnitude larger turnover frequencies. Initial C-H bond cleavage becomes more important but the general trends are similar to the vapor phase, suggesting that the reaction chemistry is similar in both vapor and aqueous phases.
Language英语
WOS IDWOS:000389224400006
Citation statistics
Cited Times:15[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/150448
Collection中国科学院大连化学物理研究所
Affiliation1.Univ South Carolina, Dept Chem Engn, 301 South Main St, Columbia, SC 29208 USA
2.Univ Engn & Technol, Dept Chem Engn, Lahore 54890, Pakistan
3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China
Recommended Citation
GB/T 7714
Faheem, Muhammad,Saleheen, Mohammad,Lu, Jianmin,et al. Ethylene glycol reforming on Pt(111): first-principles microkinetic modeling in vapor and aqueous phases[J]. Catalysis Science & Technology,2016,6(23):8242-8256.
APA Faheem, Muhammad,Saleheen, Mohammad,Lu, Jianmin,&Heyden, Andreas.(2016).Ethylene glycol reforming on Pt(111): first-principles microkinetic modeling in vapor and aqueous phases.Catalysis Science & Technology,6(23),8242-8256.
MLA Faheem, Muhammad,et al."Ethylene glycol reforming on Pt(111): first-principles microkinetic modeling in vapor and aqueous phases".Catalysis Science & Technology 6.23(2016):8242-8256.
Files in This Item:
There are no files associated with this item.
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Faheem, Muhammad]'s Articles
[Saleheen, Mohammad]'s Articles
[Lu, Jianmin]'s Articles
Baidu academic
Similar articles in Baidu academic
[Faheem, Muhammad]'s Articles
[Saleheen, Mohammad]'s Articles
[Lu, Jianmin]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Faheem, Muhammad]'s Articles
[Saleheen, Mohammad]'s Articles
[Lu, Jianmin]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.