Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale
Abstract Catalytic studies traditionally rely on steady-state conditions resulting in time-averaged datasets that do not differentiate between active and spectator species. This limitation can cause misinterpretations of catalytic function, as the signal of short-lived intermediates responsible for...
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| Format: | Article |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56576-5 |
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| author | Calley N. Eads Weijia Wang Ulrike Küst Julia Prumbs Robert H. Temperton Mattia Scardamaglia Joachim Schnadt Jan Knudsen Andrey Shavorskiy |
| author_facet | Calley N. Eads Weijia Wang Ulrike Küst Julia Prumbs Robert H. Temperton Mattia Scardamaglia Joachim Schnadt Jan Knudsen Andrey Shavorskiy |
| author_sort | Calley N. Eads |
| collection | DOAJ |
| description | Abstract Catalytic studies traditionally rely on steady-state conditions resulting in time-averaged datasets that do not differentiate between active and spectator species. This limitation can cause misinterpretations of catalytic function, as the signal of short-lived intermediates responsible for producing desired reaction products is often masked by more intense spectator species. Time-resolved ambient pressure X-ray photoelectron spectroscopy (tr-APXPS) mitigates this issue by combining microsecond time resolution under reaction conditions. Using tr-APXPS, we investigate the oxidation of CO over Pt(111) by concurrently tracking reaction products, surface intermediates, and catalyst response. Our findings reveal that chemisorbed oxygen, rather than Pt surface oxide, is the main species reacting with CO to form CO2, supporting a primary Langmuir-Hinshelwood mechanism. The results shed new light on a heavily-debated reaction in catalysis. Beyond using CO pulses to determine active species, we demonstrate how careful tuning of pulsing parameters can be used for dynamic catalyst operation to enhance CO2 formation. |
| format | Article |
| id | doaj-art-5bd278be91d6457e95bb82eecc27bfec |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-5bd278be91d6457e95bb82eecc27bfec2025-02-02T12:33:25ZengNature PortfolioNature Communications2041-17232025-01-0116111010.1038/s41467-025-56576-5Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescaleCalley N. Eads0Weijia Wang1Ulrike Küst2Julia Prumbs3Robert H. Temperton4Mattia Scardamaglia5Joachim Schnadt6Jan Knudsen7Andrey Shavorskiy8MAX IV Laboratory, Lund UniversityMAX IV Laboratory, Lund UniversityDivision of Synchrotron Radiation Research, Department of Physics, Lund UniversityDivision of Synchrotron Radiation Research, Department of Physics, Lund UniversityMAX IV Laboratory, Lund UniversityMAX IV Laboratory, Lund UniversityMAX IV Laboratory, Lund UniversityMAX IV Laboratory, Lund UniversityMAX IV Laboratory, Lund UniversityAbstract Catalytic studies traditionally rely on steady-state conditions resulting in time-averaged datasets that do not differentiate between active and spectator species. This limitation can cause misinterpretations of catalytic function, as the signal of short-lived intermediates responsible for producing desired reaction products is often masked by more intense spectator species. Time-resolved ambient pressure X-ray photoelectron spectroscopy (tr-APXPS) mitigates this issue by combining microsecond time resolution under reaction conditions. Using tr-APXPS, we investigate the oxidation of CO over Pt(111) by concurrently tracking reaction products, surface intermediates, and catalyst response. Our findings reveal that chemisorbed oxygen, rather than Pt surface oxide, is the main species reacting with CO to form CO2, supporting a primary Langmuir-Hinshelwood mechanism. The results shed new light on a heavily-debated reaction in catalysis. Beyond using CO pulses to determine active species, we demonstrate how careful tuning of pulsing parameters can be used for dynamic catalyst operation to enhance CO2 formation.https://doi.org/10.1038/s41467-025-56576-5 |
| spellingShingle | Calley N. Eads Weijia Wang Ulrike Küst Julia Prumbs Robert H. Temperton Mattia Scardamaglia Joachim Schnadt Jan Knudsen Andrey Shavorskiy Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale Nature Communications |
| title | Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale |
| title_full | Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale |
| title_fullStr | Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale |
| title_full_unstemmed | Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale |
| title_short | Resolving active species during the carbon monoxide oxidation over Pt(111) on the microsecond timescale |
| title_sort | resolving active species during the carbon monoxide oxidation over pt 111 on the microsecond timescale |
| url | https://doi.org/10.1038/s41467-025-56576-5 |
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