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题名: Ethylene glycol reforming on Pt(111): first-principles microkinetic modeling in vapor and aqueous phases
作者: Faheem, Muhammad1, 2;  Saleheen, Mohammad1;  Lu, Jianmin1, 3;  Heyden, Andreas1
刊名: Catalysis Science & Technology
发表日期: 2016
DOI: 10.1039/c6cy02111e
卷: 6, 期:23, 页:8242-8256
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
英文摘要: First-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.
关键词[WOS]: SUPPORTED PLATINUM CATALYSTS ;  FINDING SADDLE-POINTS ;  RATE-DETERMINING STEP ;  ZETA VALENCE QUALITY ;  BASIS-SETS ;  METHANOL DECOMPOSITION ;  TRANSITION-METALS ;  OXYGENATED HYDROCARBONS ;  RENEWABLE HYDROGEN ;  ENERGY
语种: 英语
WOS记录号: WOS:000389224400006
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/150448
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.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:
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.
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