Unraveling Molecular Fingerprints of Catalytic Sulfur Poisoning at the Nanometer Scale with Near-Field Infrared Spectroscopy
Artikel i vetenskaplig tidskrift, 2022

Fundamental understanding of catalytic deactivation phenomena such as sulfur poisoning occurring on metal/metal-oxide interfaces is essential for the development of high-performance heterogeneous catalysts with extended lifetimes. Unambiguous identification of catalytic poisoning species requires experimental methods simultaneously delivering accurate information regarding adsorption sites and adsorption geometries of adsorbates with nanometer-scale spatial resolution, as well as their detailed chemical structure and surface functional groups. However, to date, it has not been possible to study catalytic sulfur poisoning of metal/metal-oxide interfaces at the nanometer scale without sacrificing chemical definition. Here, we demonstrate that near-field nano-infrared spectroscopy can effectively identify the chemical nature, adsorption sites, and adsorption geometries of sulfur-based catalytic poisons on a Pd(nanodisk)/Al2O3 (thin-film) planar model catalyst surface at the nanometer scale. The current results reveal striking variations in the nature of sulfate species from one nanoparticle to another, vast alterations of sulfur poisoning on a single Pd nanoparticle as well as at the assortment of sulfate species at the active metal-metal-oxide support interfacial sites. These findings provide critical molecular-level insights crucial for the development of long-lifetime precious metal catalysts resistant toward deactivation by sulfur.

Författare

Zafer Say

Bilkent Universitesi

Chalmers, Fysik, Kemisk fysik

TOBB University of Economics and Technology

Melike Kaya

Ankara Universitesi

Turkish Accelerator and Radiation Laboratory

Çaǧll Kaderoǧlu

Ankara Universitesi

Turkish Accelerator and Radiation Laboratory

Yusuf Kocak

Bilkent Universitesi

Kerem Emre Ercan

Bilkent Universitesi

Abel Tetteh Sika-Nartey

Bilkent Universitesi

Ahsan Jalal

Bilkent Universitesi

Ahmet Arda Turk

Bilkent Universitesi

Christoph Langhammer

Chalmers, Fysik, Kemisk fysik

Mirali Jahangirzadeh Varjovi

Bilkent Universitesi

Engin Durgun

Bilkent Universitesi

Emrah Ozensoy

Bilkent Universitesi

Journal of the American Chemical Society

0002-7863 (ISSN) 1520-5126 (eISSN)

Vol. 144 19 8848-8860

Ämneskategorier

Oorganisk kemi

Materialkemi

Annan kemi

DOI

10.1021/jacs.2c03088

PubMed

35486918

Mer information

Senast uppdaterat

2024-07-23