Addition of transient kinetics capabilities to an infrared reflection absorption spectroscopy system through synchronized gas pulsing and data acquisition

Darbari, Zubin; Iloska, Marija; Bugallo, Mónica F.; Boscoboinik, J. Anibal

doi:10.1016/j.cattod.2022.05.027

Title: Addition of transient kinetics capabilities to an infrared reflection absorption spectroscopy system through synchronized gas pulsing and data acquisition

Journal Article · 21 May 2022 · Catalysis Today

DOI: https://doi.org/10.1016/j.cattod.2022.05.027 · OSTI ID:2297410

Darbari, Zubin ^[1]; Iloska, Marija ^[2]; Bugallo, Mónica F. ^[2];

^[3]

Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)

Surface science methodologies for understanding thermodynamic aspects of surface processes are at an advanced level. However, instrumentation and approaches for extracting kinetic parameters from elementary steps are far less accessible. In this work, we present an approach combining the use of a fast gas pulsing valve synchronized with data acquisition to enable surface transient kinetics studies using infrared reflection absorption spectroscopy. This methodology applies to the study of reversible processes and borrows concepts and ideas from molecular beam scattering and temporal analysis of products. Here, a temporal resolution of ~67 ms is achieved, and this is illustrated through the study of CO adsorption and desorption on a Pd(111) crystal in the presence and absence of background O₂. The same approach can be extended to other surface spectroscopies, such as X-ray photoelectron spectroscopy, to obtain spectra with high temporal resolution and signal-to-noise ratio and enable future multimodal surface transient kinetic studies aiming at elucidating reaction mechanisms.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704; SC0012573

OSTI ID:: 2297410

Report Number(s):: BNL--225289-2024-JAAM

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Vol. 417; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
CO adsorption
CO oxidation
IRAS
IRRAS
Pd(111)
RAIRS
fast surface spectroscopy
gas pulsing
infrared reflection absorption spectroscopy
surface science
transient kinetics

Title: Addition of transient kinetics capabilities to an infrared reflection absorption spectroscopy system through synchronized gas pulsing and data acquisition

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