scholarly journals Site-specific reactivity of molecules with surface defects—the case of H2 dissociation on Pt

Science ◽  
2019 ◽  
Vol 363 (6423) ◽  
pp. 155-157 ◽  
Author(s):  
Richard van Lent ◽  
Sabine V. Auras ◽  
Kun Cao ◽  
Anton J. Walsh ◽  
Michael A. Gleeson ◽  
...  

The classic system that describes weakly activated dissociation in heterogeneous catalysis has been explained by two dynamical models that are fundamentally at odds. Whereas one model for hydrogen dissociation on platinum(111) invokes a preequilibrium and diffusion toward defects, the other is based on direct and local reaction. We resolve this dispute by quantifying site-specific reactivity using a curved platinum single-crystal surface. Reactivity is step-type dependent and varies linearly with step density. Only the model that relies on localized dissociation is consistent with our results. Our approach provides absolute, site-specific reaction cross sections.

Author(s):  
H. Banzhof ◽  
I. Daberkow

A Philips EM 420 electron microscope equipped with a field emission gun and an external STEM unit was used to compare images of single crystal surfaces taken by conventional reflection electron microscopy (REM) and scanning reflection electron microscopy (SREM). In addition an angle-resolving detector system developed by Daberkow and Herrmann was used to record SREM images with the detector shape adjusted to different details of the convergent beam reflection high energy electron diffraction (CBRHEED) pattern.Platinum single crystal spheres with smooth facets, prepared by melting a thin Pt wire in an oxyhydrogen flame, served as objects. Fig. 1 gives a conventional REM image of a (111)Pt single crystal surface, while Fig. 2 shows a SREM record of the same area. Both images were taken with the (555) reflection near the azimuth. A comparison shows that the contrast effects of atomic steps are similar for both techniques, although the depth of focus of the SREM image is reduced as a result of the large illuminating aperture. But differences are observed at the lengthened images of small depressions and protrusions formed by atomic steps, which give a symmetrical contrast profile in the REM image, while an asymmetric black-white contrast is observed in the SREM micrograph. Furthermore the irregular structures which may be seen in the middle of Fig. 2 are not visible in the REM image, although it was taken after the SREM record.


Author(s):  
Niels Engholm Henriksen ◽  
Flemming Yssing Hansen

This chapter discusses a direct approach to the calculation of the rate constant k(T) that bypasses the detailed state-to-state reaction cross-sections. The method is based on the calculation of the reactive flux across a dividing surface on the potential energy surface. Versions based on classical as well as quantum mechanics are described. The classical version and its relation to Wigner’s variational theorem and recrossings of the dividing surface is discussed. Neglecting recrossings, an approximate result based on the calculation of the classical one-way flux from reactants to products is considered. Recrossings can subsequently be included via a transmission coefficient. An alternative exact expression is formulated based on a canonical average of the flux time-correlation function. It concludes with the quantum mechanical definition of the flux operator and the derivation of a relation between the rate constant and a flux correlation function.


Science ◽  
2021 ◽  
Vol 371 (6526) ◽  
pp. 260-264 ◽  
Author(s):  
Junki Tanaka ◽  
Zaihong Yang ◽  
Stefan Typel ◽  
Satoshi Adachi ◽  
Shiwei Bai ◽  
...  

The surface of neutron-rich heavy nuclei, with a neutron skin created by excess neutrons, provides an important terrestrial model system to study dilute neutron-rich matter. By using quasi-free α cluster–knockout reactions, we obtained direct experimental evidence for the formation of α clusters at the surface of neutron-rich tin isotopes. The observed monotonous decrease of the reaction cross sections with increasing mass number, in excellent agreement with the theoretical prediction, implies a tight interplay between α-cluster formation and the neutron skin. This result, in turn, calls for a revision of the correlation between the neutron-skin thickness and the density dependence of the symmetry energy, which is essential for understanding neutron stars. Our result also provides a natural explanation for the origin of α particles in α decay.


2018 ◽  
Vol 184 ◽  
pp. 02015
Author(s):  
E. Strano ◽  
M. Mazzocco ◽  
A. Boiano ◽  
C. Boiano ◽  
M. La Commara ◽  
...  

We investigated the reaction dynamics induced by the 7Be,8B+208Pb collisions at energies around the Coulomb barrier. Charged particles originated by both the col- lisions were detected by means of 6 ΔE-Eres telescopes of a newly developed detector array. Experimental data were analysed within the framework of the Optical Model and the total reaction cross-sections were compared together and with the 6,7Li+208Pb colli-sion data. According to the preliminary results, 7Be nucleus reactivity is rather similar to the 7Li one whereas the 8B+208Pb total reaction cross section appears to be much larger than those measured for reactions induced by the other weakly-bound projectiles on the same target.


2011 ◽  
Vol 84 (3) ◽  
Author(s):  
J. C. Zamora ◽  
V. Guimarães ◽  
A. Barioni ◽  
A. Lépine-Szily ◽  
R. Lichtenthäler ◽  
...  

2010 ◽  
Vol 73 (10) ◽  
pp. 1700-1706 ◽  
Author(s):  
H. Büyükuslu ◽  
A. Kaplan ◽  
A. Aydin ◽  
E. Tel ◽  
G. Yıldırım

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