Microkinetic modeling of Pt-catalyzed ethylene glycol steam reforming

被引:23
作者
Christiansen, Matthew A.
Vlachos, Dionisios G. [1 ]
机构
[1] Univ Delaware, Dept Chem & Biomol Engn, Catalysis Ctr Energy Innovat, Newark, DE 19716 USA
基金
美国国家科学基金会;
关键词
Microkinetic modeling; Platinum; Ethylene glycol; Steam reforming; DFT; BEPs; GAS-SHIFT REACTION; GROUP ADDITIVITY; PLATINUM; KINETICS; PREDICTION; METHANOL; DEHYDROGENATION; HYDROGENOLYSIS; SENSITIVITY; ADSORPTION;
D O I
10.1016/j.apcata.2012.04.010
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A predictive mean-field microkinetic model is developed for steam reforming of ethylene glycol over a Pt catalyst using a hierarchical multiscale modeling approach. The model's predictive capabilities are assessed by comparison to experimental data under kinetically controlled conditions. It is found that early dehydrogenation reaction steps control the reaction rate, highlighting a kinetic analogy between ethylene glycol steam reforming and CH4 steam reforming on Pt catalysts. (c) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:18 / 24
页数:7
相关论文
共 33 条
[21]   Density Functional Theory-Derived Group Additivity and Linear Scaling Methods for Prediction of Oxygenate Stability on Metal Catalysts: Adsorption of Open-Ring Alcohol and Polyol Dehydrogenation Intermediates on Pt-Based Metals [J].
Salciccioli, M. ;
Chen, Y. ;
Vlachos, D. G. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (47) :20155-20166
[22]   Differentiation of O-H and C-H Bond Scission Mechanisms of Ethylene Glycol on Pt and Ni/Pt Using Theory and Isotopic Labeling Experiments [J].
Salciccioli, Michael ;
Yu, Weiting ;
Barteau, Mark A. ;
Chen, Jingguang G. ;
Vlachos, Dionisios G. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (20) :7996-8004
[23]   Aqueous-phase reforming of methanol and ethylene glycol over alumina-supported platinum catalysts [J].
Shabaker, JW ;
Davda, RR ;
Huber, GW ;
Cortright, RD ;
Dumesic, JA .
JOURNAL OF CATALYSIS, 2003, 215 (02) :344-352
[24]   Glycerol as a source for fuels and chemicals by low-temperature catalytic processing [J].
Soares, Ricardo R. ;
Simonetti, Dante A. ;
Dumesic, James A. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (24) :3982-3985
[25]   The SIESTA method for ab initio order-N materials simulation [J].
Soler, JM ;
Artacho, E ;
Gale, JD ;
García, A ;
Junquera, J ;
Ordejón, P ;
Sánchez-Portal, D .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2002, 14 (11) :2745-2779
[26]   First-Principles-Based Kinetic Monte Carlo Simulation of the Structure Sensitivity of the Water-Gas Shift Reaction on Platinum Surfaces [J].
Stamatakis, Michail ;
Chen, Ying ;
Vlachos, Dionisios G. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (50) :24750-24762
[27]  
Sutton J. E., ACS CATAL UNPUB
[28]   EFFICIENT PSEUDOPOTENTIALS FOR PLANE-WAVE CALCULATIONS .2. OPERATORS FOR FAST ITERATIVE DIAGONALIZATION [J].
TROULLIER, N ;
MARTINS, JL .
PHYSICAL REVIEW B, 1991, 43 (11) :8861-8869
[29]   Beyond Petrochemicals: The Renewable Chemicals Industry [J].
Vennestrom, P. N. R. ;
Osmundsen, C. M. ;
Christensen, C. H. ;
Taarning, Esben .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (45) :10502-10509
[30]   Hierarchical multiscale model-based design of experiments, catalysts, and reactors for fuel processing [J].
Vlachos, D. G. ;
Mhadeshwar, A. B. ;
Kaisare, N. S. .
COMPUTERS & CHEMICAL ENGINEERING, 2006, 30 (10-12) :1712-1724