Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation
The attachment of molecular catalysts to conductive supports for the preparation of solid‐state anodes is important for the development of devices for electrocatalytic water oxidation. The preparation and characterization of three molecular cyclopentadienyl iridium(III) complexes, Cp*Ir(1‐pyrenyl(2‐...
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Wiley-VCH
2021
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oai:doaj.org-article:0238c44930b24c77a1643fcc73b32eb82021-11-16T03:55:58ZNoncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation2688-404610.1002/smsc.202100037https://doaj.org/article/0238c44930b24c77a1643fcc73b32eb82021-11-01T00:00:00Zhttps://doi.org/10.1002/smsc.202100037https://doaj.org/toc/2688-4046The attachment of molecular catalysts to conductive supports for the preparation of solid‐state anodes is important for the development of devices for electrocatalytic water oxidation. The preparation and characterization of three molecular cyclopentadienyl iridium(III) complexes, Cp*Ir(1‐pyrenyl(2‐pyridyl)ethanolate‐κO,κN)Cl (1) (Cp* = pentamethylcyclopentadienyl), Cp*Ir(diphenyl(2‐pyridyl)methanolate‐κO,κN)Cl (2), and [Cp*Ir(4‐(1‐pyrenyl)‐2,2′‐bipyridine)Cl]Cl (3), as precursors for electrochemical water oxidation catalysts, are reported. These complexes contain aromatic groups that can be attached via noncovalent π‐stacking to ordered mesoporous carbon (OMC). The resulting iridium‐based OMC materials (Ir‐1, Ir‐2, and Ir‐3) were tested for electrocatalytic water oxidation leading to turnover frequencies (TOFs) of 0.9–1.6 s−1 at an overpotential of 300 mV under acidic conditions. The stability of the materials is demonstrated by electrochemical cycling and X‐ray absorption spectroscopy analysis before and after catalysis. Theoretical studies on the interactions between the molecular complexes and the OMC support provide insight onto the noncovalent binding and are in agreement with the experimental loadings.Ana M. GeerChang LiuCharles B. Musgrave IIIChristopher WebberGrayson JohnsonHua ZhouCheng-Jun SunDiane A. DickieWilliam A. Goddard IIISen ZhangT. Brent GunnoeWiley-VCHarticleelectrocatalysisiridium molecular complexesnoncovalent immobilizationordered mesoporous carbonwater oxidationMaterials of engineering and construction. Mechanics of materialsTA401-492ENSmall Science, Vol 1, Iss 11, Pp n/a-n/a (2021) |
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DOAJ |
| collection |
DOAJ |
| language |
EN |
| topic |
electrocatalysis iridium molecular complexes noncovalent immobilization ordered mesoporous carbon water oxidation Materials of engineering and construction. Mechanics of materials TA401-492 |
| spellingShingle |
electrocatalysis iridium molecular complexes noncovalent immobilization ordered mesoporous carbon water oxidation Materials of engineering and construction. Mechanics of materials TA401-492 Ana M. Geer Chang Liu Charles B. Musgrave III Christopher Webber Grayson Johnson Hua Zhou Cheng-Jun Sun Diane A. Dickie William A. Goddard III Sen Zhang T. Brent Gunnoe Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation |
| description |
The attachment of molecular catalysts to conductive supports for the preparation of solid‐state anodes is important for the development of devices for electrocatalytic water oxidation. The preparation and characterization of three molecular cyclopentadienyl iridium(III) complexes, Cp*Ir(1‐pyrenyl(2‐pyridyl)ethanolate‐κO,κN)Cl (1) (Cp* = pentamethylcyclopentadienyl), Cp*Ir(diphenyl(2‐pyridyl)methanolate‐κO,κN)Cl (2), and [Cp*Ir(4‐(1‐pyrenyl)‐2,2′‐bipyridine)Cl]Cl (3), as precursors for electrochemical water oxidation catalysts, are reported. These complexes contain aromatic groups that can be attached via noncovalent π‐stacking to ordered mesoporous carbon (OMC). The resulting iridium‐based OMC materials (Ir‐1, Ir‐2, and Ir‐3) were tested for electrocatalytic water oxidation leading to turnover frequencies (TOFs) of 0.9–1.6 s−1 at an overpotential of 300 mV under acidic conditions. The stability of the materials is demonstrated by electrochemical cycling and X‐ray absorption spectroscopy analysis before and after catalysis. Theoretical studies on the interactions between the molecular complexes and the OMC support provide insight onto the noncovalent binding and are in agreement with the experimental loadings. |
| format |
article |
| author |
Ana M. Geer Chang Liu Charles B. Musgrave III Christopher Webber Grayson Johnson Hua Zhou Cheng-Jun Sun Diane A. Dickie William A. Goddard III Sen Zhang T. Brent Gunnoe |
| author_facet |
Ana M. Geer Chang Liu Charles B. Musgrave III Christopher Webber Grayson Johnson Hua Zhou Cheng-Jun Sun Diane A. Dickie William A. Goddard III Sen Zhang T. Brent Gunnoe |
| author_sort |
Ana M. Geer |
| title |
Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation |
| title_short |
Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation |
| title_full |
Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation |
| title_fullStr |
Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation |
| title_full_unstemmed |
Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation |
| title_sort |
noncovalent immobilization of pentamethylcyclopentadienyl iridium complexes on ordered mesoporous carbon for electrocatalytic water oxidation |
| publisher |
Wiley-VCH |
| publishDate |
2021 |
| url |
https://doaj.org/article/0238c44930b24c77a1643fcc73b32eb8 |
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