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Atomic insights into the competitive edge of nanosheets splitting water

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Názov: Atomic insights into the competitive edge of nanosheets splitting water
Autori: Falling, Lorenz J., Jang, Woosun, Laha, Sourav, Götsch, Thomas, Terban, Maxwell, Mom, Rik, Velasco-Vélez, Juan-Jesús, Girgsdies, Frank, Teschner, Detre, Tarasov, Andrey, Chuang, Cheng-Hao, Lunkenbein, Thomas, Knop-Gericke, Axel, Weber, Daniel, 1985, Dinnebier, Robert, Lotsch, Bettina V., Schlögl, Robert, Jones, Travis E.
Zdroj: Journal of the American Chemical Society. 146(40):27886-27902
Predmety: XPS, design rules, NEXAFS, in situ, operando, stability, electrochemistry, nanosheets, polymer electrolyte membrane (PEM), electronic structure, oxygen evolution reaction (OER), Iridium oxide
Popis: The oxygen evolution reaction (OER) provides the protons for many electrocatalytic power-to-X processes, such as the production of green hydrogen from water or methanol from CO2. Iridium oxo-hydroxides (IOHs) are outstanding catalysts for this reaction because they strike a unique balance between activity and stability in acidic electrolytes. Within IOHs, this balance varies with atomic structure. While amorphous IOHs perform best, they are least stable. The opposite is true for their crystalline counterparts. These rules-of-thumb are used to reduce the loading of scarce IOH catalysts and retain performance. However, it is not fully understood how activity and stability are related on the atomic level, hampering rational design. Herein, we provide simple design-rules (Figure 12) derived from literature and various IOHs within this study. We chose crystalline IrOOH nanosheets as our lead material because they provide excellent catalyst utilization and a predictable structure. We found that nanosheets combine the chemical stability of crystalline IOHs with the activity amorphous IOHs. Their dense bonding network of pyramidal trivalent oxygens (μ3∆–O) provides structural integrity, while allowing reversible reduction to an electronically gapped state that diminishes the destructive effect of reductive potentials. The reactivity originates from coordinative unsaturated edge sites with radical character, i.e. μ1–O oxyls. By comparing to other IOHs and literature, we generalized our findings and synthesized a set of simple rules that allow prediction of stability and reactivity of IOHs from atomistic models. We hope that these rules will inspire atomic design strategies for future OER catalysts.
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https://research.chalmers.se/publication/546608
https://research.chalmers.se/publication/543215
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  Data: Atomic insights into the competitive edge of nanosheets splitting water
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  Data: <searchLink fieldCode="AR" term="%22Falling%2C+Lorenz+J%2E%22">Falling, Lorenz J.</searchLink><br /><searchLink fieldCode="AR" term="%22Jang%2C+Woosun%22">Jang, Woosun</searchLink><br /><searchLink fieldCode="AR" term="%22Laha%2C+Sourav%22">Laha, Sourav</searchLink><br /><searchLink fieldCode="AR" term="%22Götsch%2C+Thomas%22">Götsch, Thomas</searchLink><br /><searchLink fieldCode="AR" term="%22Terban%2C+Maxwell%22">Terban, Maxwell</searchLink><br /><searchLink fieldCode="AR" term="%22Mom%2C+Rik%22">Mom, Rik</searchLink><br /><searchLink fieldCode="AR" term="%22Velasco-Vélez%2C+Juan-Jesús%22">Velasco-Vélez, Juan-Jesús</searchLink><br /><searchLink fieldCode="AR" term="%22Girgsdies%2C+Frank%22">Girgsdies, Frank</searchLink><br /><searchLink fieldCode="AR" term="%22Teschner%2C+Detre%22">Teschner, Detre</searchLink><br /><searchLink fieldCode="AR" term="%22Tarasov%2C+Andrey%22">Tarasov, Andrey</searchLink><br /><searchLink fieldCode="AR" term="%22Chuang%2C+Cheng-Hao%22">Chuang, Cheng-Hao</searchLink><br /><searchLink fieldCode="AR" term="%22Lunkenbein%2C+Thomas%22">Lunkenbein, Thomas</searchLink><br /><searchLink fieldCode="AR" term="%22Knop-Gericke%2C+Axel%22">Knop-Gericke, Axel</searchLink><br /><searchLink fieldCode="AR" term="%22Weber%2C+Daniel%22">Weber, Daniel</searchLink>, 1985<br /><searchLink fieldCode="AR" term="%22Dinnebier%2C+Robert%22">Dinnebier, Robert</searchLink><br /><searchLink fieldCode="AR" term="%22Lotsch%2C+Bettina+V%2E%22">Lotsch, Bettina V.</searchLink><br /><searchLink fieldCode="AR" term="%22Schlögl%2C+Robert%22">Schlögl, Robert</searchLink><br /><searchLink fieldCode="AR" term="%22Jones%2C+Travis+E%2E%22">Jones, Travis E.</searchLink>
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  Data: <i>Journal of the American Chemical Society</i>. 146(40):27886-27902
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  Data: <searchLink fieldCode="DE" term="%22XPS%22">XPS</searchLink><br /><searchLink fieldCode="DE" term="%22design+rules%22">design rules</searchLink><br /><searchLink fieldCode="DE" term="%22NEXAFS%22">NEXAFS</searchLink><br /><searchLink fieldCode="DE" term="%22in+situ%22">in situ</searchLink><br /><searchLink fieldCode="DE" term="%22operando%22">operando</searchLink><br /><searchLink fieldCode="DE" term="%22stability%22">stability</searchLink><br /><searchLink fieldCode="DE" term="%22electrochemistry%22">electrochemistry</searchLink><br /><searchLink fieldCode="DE" term="%22nanosheets%22">nanosheets</searchLink><br /><searchLink fieldCode="DE" term="%22polymer+electrolyte+membrane+%28PEM%29%22">polymer electrolyte membrane (PEM)</searchLink><br /><searchLink fieldCode="DE" term="%22electronic+structure%22">electronic structure</searchLink><br /><searchLink fieldCode="DE" term="%22oxygen+evolution+reaction+%28OER%29%22">oxygen evolution reaction (OER)</searchLink><br /><searchLink fieldCode="DE" term="%22Iridium+oxide%22">Iridium oxide</searchLink>
– Name: Abstract
  Label: Description
  Group: Ab
  Data: The oxygen evolution reaction (OER) provides the protons for many electrocatalytic power-to-X processes, such as the production of green hydrogen from water or methanol from CO2. Iridium oxo-hydroxides (IOHs) are outstanding catalysts for this reaction because they strike a unique balance between activity and stability in acidic electrolytes. Within IOHs, this balance varies with atomic structure. While amorphous IOHs perform best, they are least stable. The opposite is true for their crystalline counterparts. These rules-of-thumb are used to reduce the loading of scarce IOH catalysts and retain performance. However, it is not fully understood how activity and stability are related on the atomic level, hampering rational design. Herein, we provide simple design-rules (Figure 12) derived from literature and various IOHs within this study. We chose crystalline IrOOH nanosheets as our lead material because they provide excellent catalyst utilization and a predictable structure. We found that nanosheets combine the chemical stability of crystalline IOHs with the activity amorphous IOHs. Their dense bonding network of pyramidal trivalent oxygens (μ3∆–O) provides structural integrity, while allowing reversible reduction to an electronically gapped state that diminishes the destructive effect of reductive potentials. The reactivity originates from coordinative unsaturated edge sites with radical character, i.e. μ1–O oxyls. By comparing to other IOHs and literature, we generalized our findings and synthesized a set of simple rules that allow prediction of stability and reactivity of IOHs from atomistic models. We hope that these rules will inspire atomic design strategies for future OER catalysts.
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      – Type: doi
        Value: 10.1021/jacs.4c10312
    Languages:
      – Text: English
    PhysicalDescription:
      Pagination:
        PageCount: 17
        StartPage: 27886
    Subjects:
      – SubjectFull: XPS
        Type: general
      – SubjectFull: design rules
        Type: general
      – SubjectFull: NEXAFS
        Type: general
      – SubjectFull: in situ
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      – SubjectFull: operando
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      – SubjectFull: stability
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      – SubjectFull: electrochemistry
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      – SubjectFull: nanosheets
        Type: general
      – SubjectFull: polymer electrolyte membrane (PEM)
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      – SubjectFull: electronic structure
        Type: general
      – SubjectFull: oxygen evolution reaction (OER)
        Type: general
      – SubjectFull: Iridium oxide
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      – TitleFull: Atomic insights into the competitive edge of nanosheets splitting water
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