Protonengekoppelte Reduktion des katalytischen [4Fe‐4S]‐Zentrums in [FeFe]‐Hydrogenasen

Senger, Moritz; Laun, Konstantin; Wittkamp, Florian; Duan, Jifu; Haumann, Michael; Happe, Thomas; Winkler, Martin; Apfel, Ulf‐Peter; Stripp, Sven T.

doi:10.1002/ange.201709910

“…The electro‐ and photocatalytic hydrogen evolution reaction (HER) is at the heart of a H 2 ‐based new energy society . In nature, hydrogenases can mediate the reversible H 2 /H + conversion, but the use of these enzymes suffer from difficulties in their scale‐up preparation and also from their inactivation under aerobic conditions . As a result, developing HER catalysts that are cheap, efficient, and robust has attracted increasing interests …”

Section: Figurementioning

confidence: 99%

Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Xie

¹

,

Tian

²

,

Ouyang

³

et al. 2020

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Molecular design to improve catalyst performance is significant but challenging. In enzymes, residue groups that are close to reaction centers play critical roles in regulating activities. Using this bioinspired strategy, three water‐soluble polymers were designed with appending Co porphyrins and different side‐chain groups to mimic enzyme reaction centers and activity‐controlling residue groups, respectively. With these polymers, high hydrogen evolution efficiency was achieved in neutral aqueous media for electro‐ (turnover frequency >2.3×104 s−1) and photocatalysis (turnover number >2.7×104). Porphyrin units are surrounded and protected by polymer chains, and more importantly, the activity can be tuned with different side‐chain groups. Therefore, instead of revising molecular structures that is difficult from both design and synthesis points of view, polymers can be used to improve molecular solubility and stability and simultaneously regulate activity by using side‐chain groups.

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“…The electro‐ and photocatalytic hydrogen evolution reaction (HER) is at the heart of a H 2 ‐based new energy society . In nature, hydrogenases can mediate the reversible H 2 /H + conversion, but the use of these enzymes suffer from difficulties in their scale‐up preparation and also from their inactivation under aerobic conditions . As a result, developing HER catalysts that are cheap, efficient, and robust has attracted increasing interests …”

Section: Figurementioning

confidence: 99%

Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Xie

¹

,

Tian

²

,

Ouyang

³

et al. 2020

Self Cite

View full text Add to dashboard Cite

Molecular design to improve catalyst performance is significant but challenging. In enzymes, residue groups that are close to reaction centers play critical roles in regulating activities. Using this bioinspired strategy, three water‐soluble polymers were designed with appending Co porphyrins and different side‐chain groups to mimic enzyme reaction centers and activity‐controlling residue groups, respectively. With these polymers, high hydrogen evolution efficiency was achieved in neutral aqueous media for electro‐ (turnover frequency >2.3×104 s−1) and photocatalysis (turnover number >2.7×104). Porphyrin units are surrounded and protected by polymer chains, and more importantly, the activity can be tuned with different side‐chain groups. Therefore, instead of revising molecular structures that is difficult from both design and synthesis points of view, polymers can be used to improve molecular solubility and stability and simultaneously regulate activity by using side‐chain groups.

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ADUC‐Preise: U.‐P. Apfel, P. Heretsch, O. Hollóczki / Carl‐Duisberg‐Gedächtnispreis: B. Morandi / Neu in der Académie des Sciences: E. Charpentier, J. Cossy, I. Marek / Max‐Delbrück‐Nachwuchspreis: S. Disch / Novartis Early Career Award: B. Morandi und R. R. Knowles

2018

Angewandte Chemie

10

0

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Protonengekoppelte Reduktion des katalytischen [4Fe‐4S]‐Zentrums in [FeFe]‐Hydrogenasen

Abstract: In der Natur katalysieren [FeFe]-Hydrogenasen die

Cited by 7 publications

References 43 publications

Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

Water‐Soluble Polymers with Appending Porphyrins as Bioinspired Catalysts for the Hydrogen Evolution Reaction

ADUC‐Preise: U.‐P. Apfel, P. Heretsch, O. Hollóczki / Carl‐Duisberg‐Gedächtnispreis: B. Morandi / Neu in der Académie des Sciences: E. Charpentier, J. Cossy, I. Marek / Max‐Delbrück‐Nachwuchspreis: S. Disch / Novartis Early Career Award: B. Morandi und R. R. Knowles

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