The role of steps in the dynamics of hydrogen dissociation on Pt(533)

The dissociative adsorption of H2 and D2 on Pt(533) (Pt{4(111)×(100)}) has been investigated using temperature programmed desorption and supersonic molecular beams. Associative desorption of D2 from (100) step sites is observed at lowest exposures in TPD (assigned β3) at 375 K. Saturation of this peak at ΘH=0.14 corresponds to the filling of half of the available four-fold sites at the (100) step edge. At higher coverages, additional desorption takes place from the (111) terraces in a broad peak below 300 K similar to that observed (assigned β1 and β2) for the Pt(111) surface. The incident kinetic energy (Ei), surface temperature (Ts), coverage (ΘD), and incident angle (Φ) dependence of the dissociative sticking probability (S) was also measured. The initial dissociative sticking probability (S0) first decreases with increasing kinetic energy over the range 0<Ei(meV)<150 (low energy component), and subsequently increases (high energy component). Comparison with D2 dissociation on Pt(111), where (S0) incre...

[1]  B. Hayden,et al.  The mechanism of sticking trapping and direct dissociation of carbon monoxide on Cu(110) , 1990 .

[2]  G. Ertl,et al.  Interaction of hydrogen with Pt(111): The role of atomic steps , 1976 .

[3]  B. Poelsema,et al.  Temperature dependency of the initial sticking probability of H2 and CO on Pt(111) , 1985 .

[4]  A. Luntz,et al.  Molecular beam studies of H2 and D2 dissociative chemisorption on Pt(111) , 1990 .

[5]  A. Rar,et al.  Desorption and dissociation of oxygen admolecules on a stepped platinum (533) surface , 1994 .

[6]  Müller Je Model of an H2-precursor state on metal surfaces. , 1987 .

[7]  A. Baró,et al.  Vibrational modes of hydrogen adsorbed on Pt(111): Adsorption site and excitation mechanism , 1979 .

[8]  S. Holloway,et al.  How far can classical mechanics be trusted when treating surface reactions , 1996 .

[9]  K. Svensson,et al.  Adsorption of hydrogen on stepped Ni and Pd surfaces - observation of chemisorbed hydrogen molecules , 1993 .

[10]  B. Hayden,et al.  The indirect channel to hydrogen dissociation on W(100)-c(2×2)Cu. Evidence for a dynamical precursor , 1995 .

[11]  Winkler,et al.  Adsorption probabilities of H2 and D2 on various flat and stepped nickel surfaces. , 1985, Physical review. B, Condensed matter.

[12]  J. Harris,et al.  Recoil effects in surface dissociation , 1990 .

[13]  A. Gross Quantum effects in the dissociative adsorption of hydrogen , 1999 .

[14]  A. Winkler,et al.  Wide range nozzle beam adsorption data for the systems H2/nickel and H2/Pd(100) , 1989 .

[15]  B. Poelsema,et al.  A molecular beam study of the interaction between hydrogen and the Pt(111) surface , 1989 .

[16]  A. Winkler,et al.  Adsorption of hydrogen on tungsten: a precursor path plus direct adsorption , 1992 .

[17]  Ab initio quantum and molecular dynamics of the dissociative adsorption of hydrogen on Pd(100) , 1997, cond-mat/9705102.

[18]  J. A. White,et al.  STEERING EFFECTS IN NON-ACTIVATED ADSORPTION , 1995 .

[19]  D. King,et al.  Molecular Beam Investigation of Adsorption Kinetics on Bulk Metal Targets: Nitrogen on Tungsten , 1972 .

[20]  G. Somorjai,et al.  A modulated molecular beam study of the mechanism of the H2–D2 exchange reaction on Pt(111) and Pt(332) crystal surfaces , 1979 .

[21]  S. Holloway,et al.  Comparing quantum and classical dynamics: H2 dissociation on W(100) , 1998 .

[22]  G. Somorjai,et al.  MOLECULAR BEAM STUDY OF THE MECHANISM OF CATALYZED HYDROGEN-DEUTERIUM EXCHANGE ON PLATINUM SINGLE CRYSTAL SURFACES , 1975 .

[23]  G. Ertl,et al.  Adsorption of hydrogen on a Pt(111) surface , 1976 .

[24]  B. Koel,et al.  Deuterium dissociation on ordered Sn/Pt(111) surface alloys , 1998 .

[25]  B. Hayden,et al.  Precursor dynamics in dissociative hydrogen adsorption on W (100) , 1994 .

[26]  Six-dimensional quantum dynamics of adsorption and desorption of H2 at Pd(100): Steering and steric effects. , 1995, Physical review letters.

[27]  S. Holloway,et al.  The steering of molecules in simple dissociation reactions , 1998 .

[28]  B. Hayden,et al.  Vibrational and translational energy partition and the barrier to dissociative H2 and D2 adsorption on Cu(110) , 1991 .

[29]  B. Hayden,et al.  Dynamics of direct and indirect channels to dissociative adsorption , 1994 .

[30]  E. Bertel Electronic surface states and the hydrogen dissociation barrier , 1997 .

[31]  A. Winkler,et al.  Adsorption kinetics for hydrogen adsorption on nickel and coadsorption of hydrogen and oxygen , 1982 .

[32]  A. Winkler,et al.  Microfacets of the (1 × 2) reconstructed Pt(110) surface seen in the adsorption dynamics of H2 , 1989 .

[33]  White,et al.  Dissociation of H2 on W(100). , 1996, Physical review. B, Condensed matter.

[34]  C. Rettner,et al.  Search for oscillations in the translational energy dependence of the dissociation of H2 on Pd(100) , 1996 .

[35]  K. Rendulic,et al.  Adsorption dynamics for the system hydrogen/palladium and its relation to the surface electronic structure , 1994 .

[36]  G. Somorjai,et al.  Molecular beam study of the H2–D2 exchange reaction on stepped platinum crystal surfaces: Dependence on reactant angle of incidence , 1977 .

[37]  J. Müller Interaction of H2O, CO, and H2 with Pt(111) and Pt(111)+K surfaces , 1989 .

[38]  M. Salmeron,et al.  VARIATION OF SURFACE REACTION PROBABILITY WITH REACTANT ANGLE OF INCIDENCE. A MOLECULAR BEAM STUDY OF THE ASYMMETRY OF STEPPED PLATINUM CRYSTAL SURFACES FOR H-H BOND BREAKING , 1977 .