Prediction of Mode Specificity, Bond Selectivity, Normal Scaling, and Surface Lattice Effects in Water Dissociative Chemisorption on Several Metal Surfaces Using the Sudden Vector Projection Model

被引:31
作者
Jiang, Bin [1 ]
Guo, Hua [1 ]
机构
[1] Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA
基金
美国国家科学基金会;
关键词
GAS SHIFT REACTION; DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; ELASTIC BAND METHOD; C-H STRETCH; PT(110)-(1 X-2); MOLECULAR-BEAM; METHANE; NI(111); CH4;
D O I
10.1021/jp5090839
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
Dissociative chemisorption of water is a key step in many heterogeneous catalytic processes such as watergas shift and steam reformation. As a result, a better understanding of the mechanism and dynamics of these processes is important for developing a predictive model of catalysis. In this work, we use the recently proposed Sudden Vector Projection (SVP) model to predict mode specificity, bond selectivity, normal scaling behavior, and surface lattice effects in water dissociative chemisorption on Ni(111), Cu(111), Pt(111), and Pt(110)-(1 x 2), based on direct plane-wave density functional theory calculations. While mode specificity and bond selectivity are similar on these surfaces, the SVP model predicts significant differences in the reaction promoting effects of kinetic energies in the surface normal and along the surface plane, signifying the different characters of the transition state on these metal surfaces. Furthermore, the involvement of surface atoms is shown, which predicts significant surface temperature effects.
引用
收藏
页码:26851 / 26858
页数:8
相关论文
共 67 条
[1]  
[Anonymous], 2005, STAND HDB CHAINS
[2]  
Beck R. D., 2013, DYNAMICS OF GAS SURF
[3]   Vibrational mode-specific reaction of methane on a nickel surface [J].
Beck, RD ;
Maroni, P ;
Papageorgopoulos, DC ;
Dang, TT ;
Schmid, MP ;
Rizzo, TR .
SCIENCE, 2003, 302 (5642) :98-100
[4]   State-resolved reactivity of CH4(2ν3) on Pt(111) and Ni(111):: Effects of barrier height and transition state location [J].
Bisson, R. ;
Sacchi, M. ;
Dang, T. T. ;
Yoder, B. ;
Maroni, P. ;
Beck, R. D. .
JOURNAL OF PHYSICAL CHEMISTRY A, 2007, 111 (49) :12679-12683
[5]   Computational Investigation of Thermochemistry and Kinetics of Steam Methane Reforming on Ni(111) under Realistic Conditions [J].
Blaylock, D. Wayne ;
Ogura, Teppei ;
Green, William H. ;
Beran, Gregory J. O. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (12) :4898-4908
[6]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[7]   DFT Study of the Water-Gas Shift Reaction and Coke Formation on Ni(111) and Ni(211) Surfaces [J].
Catapan, Rafael C. ;
Oliveira, Amir A. M. ;
Chen, Ying ;
Vlachos, Dionisios G. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (38) :20281-20291
[8]   Vibrationally bond-selected chemisorption of methane isotopologues on Pt(111) studied by reflection absorption infrared spectroscopy [J].
Chen, Li ;
Ueta, Hirokazu ;
Bisson, Regis ;
Beck, Rainer D. .
FARADAY DISCUSSIONS, 2012, 157 :285-295
[9]  
Chorkendorff I, 2003, CONCEPTS OF MODERN C
[10]   Vibrational state dependence of D-2 dissociation on Ag(111) [J].
Cottrell, C ;
Carter, RN ;
Nesbitt, A ;
Samson, P ;
Hodgson, A .
JOURNAL OF CHEMICAL PHYSICS, 1997, 106 (11) :4714-4722