Revealing CO2 dissociation pathways at vicinal copper (997) interfaces
Abstract Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO2) activation. Despite extensive reactivity benchmarks, a correlation between CO2 conversion and morphology structure has not yet been established at vicinal Cu interfaces. Herein, ambien...
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| Format: | Article |
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Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38928-1 |
| _version_ | 1797806627890397184 |
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| author | Jeongjin Kim Youngseok Yu Tae Won Go Jean-Jacques Gallet Fabrice Bournel Bongjin Simon Mun Jeong Young Park |
| author_facet | Jeongjin Kim Youngseok Yu Tae Won Go Jean-Jacques Gallet Fabrice Bournel Bongjin Simon Mun Jeong Young Park |
| author_sort | Jeongjin Kim |
| collection | DOAJ |
| description | Abstract Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO2) activation. Despite extensive reactivity benchmarks, a correlation between CO2 conversion and morphology structure has not yet been established at vicinal Cu interfaces. Herein, ambient pressure scanning tunneling microscopy reveals step-broken Cu nanocluster evolutions on the Cu(997) surface under 1 mbar CO2(g). The CO2 dissociation reaction produces carbon monoxide (CO) adsorbate and atomic oxygen (O) at Cu step-edges, inducing complicated restructuring of the Cu atoms to compensate for increased surface chemical potential energy at ambient pressure. The CO molecules bound at under-coordinated Cu atoms contribute to the reversible Cu clustering with the pressure gap effect, whereas the dissociated oxygen leads to irreversible Cu faceting geometries. Synchrotron-based ambient pressure X-ray photoelectron spectroscopy identifies the chemical binding energy changes in CO-Cu complexes, which proves the characterized real-space evidence for the step-broken Cu nanoclusters under CO(g) environments. Our in situ surface observations provide a more realistic insight into Cu nanocatalyst designs for efficient CO2 conversion to renewable energy sources during C1 chemical reactions. |
| first_indexed | 2024-03-13T06:10:09Z |
| format | Article |
| id | doaj.art-24efa8620a034d5f9fb01ad55ee16847 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T06:10:09Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-24efa8620a034d5f9fb01ad55ee168472023-06-11T11:19:04ZengNature PortfolioNature Communications2041-17232023-06-0114111010.1038/s41467-023-38928-1Revealing CO2 dissociation pathways at vicinal copper (997) interfacesJeongjin Kim0Youngseok Yu1Tae Won Go2Jean-Jacques Gallet3Fabrice Bournel4Bongjin Simon Mun5Jeong Young Park6Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Department of Physics and Photon Science, School of Physics and Chemistry, Gwangju Institute of Science and Technology (GIST)Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Laboratoire de Chimie Physique-Matière et Rayonnement, CNRS, Sorbonne UniversitéLaboratoire de Chimie Physique-Matière et Rayonnement, CNRS, Sorbonne UniversitéDepartment of Physics and Photon Science, School of Physics and Chemistry, Gwangju Institute of Science and Technology (GIST)Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Abstract Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO2) activation. Despite extensive reactivity benchmarks, a correlation between CO2 conversion and morphology structure has not yet been established at vicinal Cu interfaces. Herein, ambient pressure scanning tunneling microscopy reveals step-broken Cu nanocluster evolutions on the Cu(997) surface under 1 mbar CO2(g). The CO2 dissociation reaction produces carbon monoxide (CO) adsorbate and atomic oxygen (O) at Cu step-edges, inducing complicated restructuring of the Cu atoms to compensate for increased surface chemical potential energy at ambient pressure. The CO molecules bound at under-coordinated Cu atoms contribute to the reversible Cu clustering with the pressure gap effect, whereas the dissociated oxygen leads to irreversible Cu faceting geometries. Synchrotron-based ambient pressure X-ray photoelectron spectroscopy identifies the chemical binding energy changes in CO-Cu complexes, which proves the characterized real-space evidence for the step-broken Cu nanoclusters under CO(g) environments. Our in situ surface observations provide a more realistic insight into Cu nanocatalyst designs for efficient CO2 conversion to renewable energy sources during C1 chemical reactions.https://doi.org/10.1038/s41467-023-38928-1 |
| spellingShingle | Jeongjin Kim Youngseok Yu Tae Won Go Jean-Jacques Gallet Fabrice Bournel Bongjin Simon Mun Jeong Young Park Revealing CO2 dissociation pathways at vicinal copper (997) interfaces Nature Communications |
| title | Revealing CO2 dissociation pathways at vicinal copper (997) interfaces |
| title_full | Revealing CO2 dissociation pathways at vicinal copper (997) interfaces |
| title_fullStr | Revealing CO2 dissociation pathways at vicinal copper (997) interfaces |
| title_full_unstemmed | Revealing CO2 dissociation pathways at vicinal copper (997) interfaces |
| title_short | Revealing CO2 dissociation pathways at vicinal copper (997) interfaces |
| title_sort | revealing co2 dissociation pathways at vicinal copper 997 interfaces |
| url | https://doi.org/10.1038/s41467-023-38928-1 |
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