Issue 31, 2020

Quantum state and surface-site-resolved studies of methane chemisorption by vibrational spectroscopies

Abstract

-The combination of quantum state-specific reactant preparation by infrared laser pumping with surface-site-resolved detection of chemisorbed reaction products by Reflection Absorption Infrared Spectroscopy (RAIRS) enables highly detailed studies of molecule/surface reactivity. In this perspective, we review the methodologies developed for simultaneous quantumstate and surface-site-resolved reactivity measurements and their application towards the chemisorption of methane on stepped and kinked platinum surfaces. We demonstrate that RAIRS allows for surface-site-resolved detection of methane dissociation, which serves to measure surface-site-resolved product uptake curves, sticking probabilities, and dissociation barrier heights. For the dissociation of C–H stretch excited singly deuterated CH3D on a stepped Pt surface such as Pt(211), RAIRS was used to detect bond selectivity in methane chemisorption and to reveal how the bond-selective dissociation proceeds from the step to the terrace sites with increasing incident kinetic energy of the CH3D reactant. Extension to site-selective RAIRS detection of methane dissociation to other vicinal surfaces such as Pt(210), Pt(531), and Pt(110)-(2 × 1) is also presented.

Graphical abstract: Quantum state and surface-site-resolved studies of methane chemisorption by vibrational spectroscopies

Article information

Article type
Perspective
Submitted
11 Jun. 2020
Accepted
16 Jul. 2020
First published
29 Jul. 2020

Phys. Chem. Chem. Phys., 2020,22, 17448-17459

Quantum state and surface-site-resolved studies of methane chemisorption by vibrational spectroscopies

A. Gutiérrez-González and R. D. Beck, Phys. Chem. Chem. Phys., 2020, 22, 17448 DOI: 10.1039/D0CP03134H

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