Fundamental Structural and Electronic Understanding of Palladium Catalysts on Nitride and Oxide Supports
© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH..
The nature of the support can fundamentally affect the function of a heterogeneous catalyst. For the novel type of isolated metal atom catalysts, sometimes referred to as single-atom catalysts, systematic correlations are still rare. Here, we report a general finding that Pd on nitride supports (non-metal and metal nitride) features a higher oxidation state compared to that on oxide supports (non-metal and metal oxide). Through thorough oxidation state investigations by X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), CO-DRIFTS, and density functional theory (DFT) coupled with Bader charge analysis, it is found that Pd atoms prefer to interact with surface hydroxyl group to form a Pd(OH)x species on oxide supports, while on nitride supports, Pd atoms incorporate into the surface structure in the form of Pd-N bonds. Moreover, a correlation was built between the formal oxidation state and computational Bader charge, based on the periodic trend in electronegativity.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - year:2024 |
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| Enthalten in: |
Angewandte Chemie (International ed. in English) - (2024) vom: 11. März, Seite e202400174 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Huang, Junhao [VerfasserIn] |
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Date Revised 09.04.2024 published: Print-Electronic Citation Status Publisher |
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| doi: |
10.1002/anie.202400174 |
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| PPN (Katalog-ID): |
NLM369565347 |
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| 520 | |a © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. | ||
| 520 | |a The nature of the support can fundamentally affect the function of a heterogeneous catalyst. For the novel type of isolated metal atom catalysts, sometimes referred to as single-atom catalysts, systematic correlations are still rare. Here, we report a general finding that Pd on nitride supports (non-metal and metal nitride) features a higher oxidation state compared to that on oxide supports (non-metal and metal oxide). Through thorough oxidation state investigations by X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), CO-DRIFTS, and density functional theory (DFT) coupled with Bader charge analysis, it is found that Pd atoms prefer to interact with surface hydroxyl group to form a Pd(OH)x species on oxide supports, while on nitride supports, Pd atoms incorporate into the surface structure in the form of Pd-N bonds. Moreover, a correlation was built between the formal oxidation state and computational Bader charge, based on the periodic trend in electronegativity | ||
| 650 | 4 | |a Journal Article | |
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| 700 | 1 | |a Tian, Xinxin |e verfasserin |4 aut | |
| 700 | 1 | |a Bartling, Stephan |e verfasserin |4 aut | |
| 700 | 1 | |a Zimina, Anna |e verfasserin |4 aut | |
| 700 | 1 | |a Radtke, Martin |e verfasserin |4 aut | |
| 700 | 1 | |a Rockstroh, Nils |e verfasserin |4 aut | |
| 700 | 1 | |a Naliwajko, Pawel |e verfasserin |4 aut | |
| 700 | 1 | |a Steinfeldt, Norbert |e verfasserin |4 aut | |
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