Redox properties of birnessite from a defect perspective
Birnessite, a layered-structure MnO2, is an earth-abundant functional material with potential for various energy and environmental applications, such as water oxidation. An important feature of birnessite is the existence of Mn(III) within the MnO2 layers, accompanied by interlayer charge-neutralizing cations. Using first-principles calculations, we reveal the nature of Mn(III) in birnessite with the concept of the small polaron, a special kind of point defect. Further taking into account the effect of the spatial distribution of Mn(III), we propose a theoretical model to explain the structure--performance dependence of birnessite as an oxygen evolution catalyst. We find an internal potential step which leads to the easy switching of the oxidation state between Mn(III) and Mn(IV) that is critical for enhancing the catalytic activity of birnessite. Finally, we conduct a series of comparative experiments which support our model..
| Medienart: |
Artikel |
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| Erscheinungsjahr: |
2017 |
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| Erschienen: |
2017 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:114 |
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| Enthalten in: |
Proceedings of the National Academy of Sciences of the United States of America - 114(2017), 36, Seite 9523 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Peng, Haowei [VerfasserIn] |
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| Links: |
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| doi: |
10.1073/pnas.1706836114 |
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| Förderinstitution / Projekttitel: |
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OLC1998536467 |
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| 520 | |a Birnessite, a layered-structure MnO2, is an earth-abundant functional material with potential for various energy and environmental applications, such as water oxidation. An important feature of birnessite is the existence of Mn(III) within the MnO2 layers, accompanied by interlayer charge-neutralizing cations. Using first-principles calculations, we reveal the nature of Mn(III) in birnessite with the concept of the small polaron, a special kind of point defect. Further taking into account the effect of the spatial distribution of Mn(III), we propose a theoretical model to explain the structure--performance dependence of birnessite as an oxygen evolution catalyst. We find an internal potential step which leads to the easy switching of the oxidation state between Mn(III) and Mn(IV) that is critical for enhancing the catalytic activity of birnessite. Finally, we conduct a series of comparative experiments which support our model. | ||
| 650 | 4 | |a Oxide minerals | |
| 650 | 4 | |a Oxidation-reduction reaction | |
| 650 | 4 | |a Observations | |
| 650 | 4 | |a Chemical properties | |
| 650 | 4 | |a Redox properties | |
| 650 | 4 | |a Switching | |
| 650 | 4 | |a Spatial distribution | |
| 650 | 4 | |a Catalytic activity | |
| 650 | 4 | |a Studies | |
| 650 | 4 | |a Manganese compounds | |
| 650 | 4 | |a Manganese oxides | |
| 650 | 4 | |a Valence | |
| 650 | 4 | |a Cations | |
| 650 | 4 | |a Interlayers | |
| 650 | 4 | |a Oxidation | |
| 650 | 4 | |a Chemical evolution | |
| 650 | 4 | |a Manganese | |
| 650 | 4 | |a Spatial discrimination | |
| 650 | 4 | |a Catalysis | |
| 700 | 1 | |a McKendry, Ian G |4 oth | |
| 700 | 1 | |a Ding, Ran |4 oth | |
| 700 | 1 | |a Thenuwara, Akila C |4 oth | |
| 700 | 1 | |a Kang, Qing |4 oth | |
| 700 | 1 | |a Shumlas, Samantha L |4 oth | |
| 700 | 1 | |a Strongin, Daniel R |4 oth | |
| 700 | 1 | |a Zdilla, Michael J |4 oth | |
| 700 | 1 | |a Perdew, and John P |4 oth | |
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| 773 | 1 | 8 | |g volume:114 |g year:2017 |g number:36 |g pages:9523 |
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