Detail publikace
Identical Fe-N4 Sites with Different Reactivity: Elucidating the Effect of Support Curvature
JAKUB, Z. PLANER, J. HRŮZA, D. TRLLOVÁ SHAHSAVAR, A. PAVELEC, J. ČECHAL, J.
Originální název
Identical Fe-N4 Sites with Different Reactivity: Elucidating the Effect of Support Curvature
Typ
článek v časopise ve Web of Science, Jimp
Jazyk
angličtina
Originální abstrakt
Detailed atomic-scale understanding is a crucial prerequisite for rational design of next-generation single-atom catalysts (SACs). However, the sub-& aring;ngstrom precision needed for systematic studies is challenging to achieve on common SACs. Here, we present a two-dimensional (2D) metal-organic system featuring Fe-N4 single-atom sites, where the metal-organic structure is modulated by 0.4 & Aring; corrugation of an inert graphene/Ir(111) support. Using scanning tunneling microscopy and density functional theory, we show that the support corrugation significantly affects the reactivity of the system, as the sites above the support "valleys" bind TCNQ (tetracyanoquinodimethane) significantly stronger than the sites above the "hills". The experimental temperature stability of TCNQ varies by more than 60 degrees C, while computations indicate more than 0.3 eV variation of TCNQ adsorption energy across the Fe-N4 sites placed atop different regions of the corrugated graphene unit cell. The origin of this effect is steric hindrance, which plays a role whenever large molecules interact with neighboring single-atom catalyst sites or when multiple reactants coadsorb on such sites. Our work demonstrates that such effects can be quantitatively studied using model SAC systems supported on chemically inert and physically corrugated supports.
Klíčová slova
single atom catalysis; 2D metal-organic frameworks; scanning tunneling microscopy; density functional theory; adsorption; Fe-N4 site
Autoři
JAKUB, Z.; PLANER, J.; HRŮZA, D.; TRLLOVÁ SHAHSAVAR, A.; PAVELEC, J.; ČECHAL, J.
Vydáno
29. 1. 2025
Nakladatel
AMER CHEMICAL SOC
Místo
WASHINGTON
ISSN
1944-8252
Periodikum
ACS applied materials & interfaces
Ročník
17
Číslo
6
Stát
Spojené státy americké
Strany od
10136
Strany do
10144
Strany počet
9
URL
BibTex
@article{BUT198066,
author="Zdeněk {Jakub} and Jakub {Planer} and Dominik {Hrůza} and Jiří {Pavelec} and Jan {Čechal} and Azin {Trllová Shahsavar}",
title="Identical Fe-N4 Sites with Different Reactivity: Elucidating the Effect of Support Curvature",
journal="ACS applied materials & interfaces",
year="2025",
volume="17",
number="6",
pages="10136--10144",
doi="10.1021/acsami.4c19913",
issn="1944-8252",
url="https://pubs.acs.org/doi/10.1021/acsami.4c19913"
}