Probing Catalytic Sites and Adsorbate Spillover on Ultrathin FeO2-x Film on Ir(111) during CO Oxidation
The spatially resolved identification of active sites on the heterogeneous catalyst surface is an essential step toward directly visualizing a catalytic reaction with atomic scale. To date, ferrous centers on platinum group metals have shown promising potential for low-temperature CO catalytic oxidation, but the temporal and spatial distribution of active sites during the reaction and how molecular-scale structures develop at the interface are not fully understood. Here, we studied the catalytic CO oxidation and the effect of co-adsorbed hydrogen on the FeO2-x/Ir(111) surface. Combining scanning tunneling microscopy (STM), isotope-labeled pulse reaction measurements, and DFT calculations, we identified both FeO2/Ir and FeO2/FeO sites as active sites with different reactivity. The trilayer O-Fe-O structure with its Moiré pattern can be fully recovered after O2 exposure, where molecular O2 dissociates at the FeO/Ir interface. Additionally, as a competitor, dissociated hydrogen migrates onto the oxide film with the formation of surface hydroxyl and water clusters down to 150 K.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2024 |
|---|---|
| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:18 |
|---|---|
| Enthalten in: |
ACS nano - 18(2024), 9 vom: 05. März, Seite 7114-7122 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Yin, Hao [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
CO oxidation |
|---|
| Anmerkungen: |
Date Revised 09.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
|---|
| doi: |
10.1021/acsnano.3c11400 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM36867617X |
|---|
| LEADER | 01000caa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM36867617X | ||
| 003 | DE-627 | ||
| 005 | 20240309232315.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 240222s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1021/acsnano.3c11400 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1321.xml |
| 035 | |a (DE-627)NLM36867617X | ||
| 035 | |a (NLM)38377596 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Yin, Hao |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Probing Catalytic Sites and Adsorbate Spillover on Ultrathin FeO2-x Film on Ir(111) during CO Oxidation |
| 264 | 1 | |c 2024 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a ƒaComputermedien |b c |2 rdamedia | ||
| 338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Date Revised 09.03.2024 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a The spatially resolved identification of active sites on the heterogeneous catalyst surface is an essential step toward directly visualizing a catalytic reaction with atomic scale. To date, ferrous centers on platinum group metals have shown promising potential for low-temperature CO catalytic oxidation, but the temporal and spatial distribution of active sites during the reaction and how molecular-scale structures develop at the interface are not fully understood. Here, we studied the catalytic CO oxidation and the effect of co-adsorbed hydrogen on the FeO2-x/Ir(111) surface. Combining scanning tunneling microscopy (STM), isotope-labeled pulse reaction measurements, and DFT calculations, we identified both FeO2/Ir and FeO2/FeO sites as active sites with different reactivity. The trilayer O-Fe-O structure with its Moiré pattern can be fully recovered after O2 exposure, where molecular O2 dissociates at the FeO/Ir interface. Additionally, as a competitor, dissociated hydrogen migrates onto the oxide film with the formation of surface hydroxyl and water clusters down to 150 K | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a CO oxidation | |
| 650 | 4 | |a hydrogen spillover | |
| 650 | 4 | |a iron oxides | |
| 650 | 4 | |a model catalyst | |
| 650 | 4 | |a surface science | |
| 700 | 1 | |a Yan, Yu-Wei |e verfasserin |4 aut | |
| 700 | 1 | |a Fang, Wei |e verfasserin |4 aut | |
| 700 | 1 | |a Brune, Harald |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t ACS nano |d 2007 |g 18(2024), 9 vom: 05. März, Seite 7114-7122 |w (DE-627)NLM18248100X |x 1936-086X |7 nnns |
| 773 | 1 | 8 | |g volume:18 |g year:2024 |g number:9 |g day:05 |g month:03 |g pages:7114-7122 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1021/acsnano.3c11400 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 18 |j 2024 |e 9 |b 05 |c 03 |h 7114-7122 | ||