Poly(dehydroalanine)-Based Hydrogels as Efficient Soft Matter Matrices for Light-Driven Catalysis

Publikationstyp:
Zeitschriftenaufsatz
Metadaten:
Autoren
  • Tolga Ceper
  • Marcel Langer
  • Nikita Vashistha
  • Benjamin Dietzek-Ivansic
  • Carsten Streb
  • Sven Rau
  • Felix H Schacher
Autoren-URL
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:001150523200001&DestLinkType=FullRecord&DestApp=WOS_CPL
DOI
10.1002/marc.202300448
eISSN
1521-3927
Externe Identifier
  • Clarivate Analytics Document Solution ID: KC9S4
  • PubMed Identifier: 38232973
ISSN
1022-1336
Ausgabe der Veröffentlichung
5
Zeitschrift
MACROMOLECULAR RAPID COMMUNICATIONS
Schlüsselwörter
  • artificial photosynthesis
  • energy-conversion
  • hydrogen evolution reaction
  • oxygen evolution reaction
  • polyampholyte hydrogel scaffold
  • visible light-driven catalysis
Datum der Veröffentlichung
2024
Status
Published
Titel
Poly(dehydroalanine)-Based Hydrogels as Efficient Soft Matter Matrices for Light-Driven Catalysis
Sub types
  • Article
Ausgabe der Zeitschrift
45

Datenquelle: Web of Science (Lite)

Andere Metadatenquellen:
Abstract
<jats:title>Abstract</jats:title><jats:p>Soft matter integration of photosensitizers and catalysts provides promising solutions to developing sustainable materials for energy conversion. Particularly, hydrogels bring unique benefits, such as spatial control and 3D‐accessibility of molecular units, as well as recyclability. Herein, the preparation of polyampholyte hydrogels based on poly(dehydroalanine) (PDha) is reported. Chemically crosslinked PDha with bis‐epoxy poly(ethylene glycol) leads to a transparent, self‐supporting hydrogel. Due to the ionizable groups on PDha, this 3D polymeric matrix can be anionic, cationic, or zwitterionic depending on the pH value, and its high density of dynamic charges has a potential for electrostatic attachment of charged molecules. The integration of the cationic molecular photosensitizer [Ru(bpy)<jats:sub>3</jats:sub>]<jats:sup>2+</jats:sup> (bpy = 2,2′‐bipyridine) is realized, which is a reversible process controlled by pH, leading to light harvesting hydrogels. They are further combined with either a thiomolybdate catalyst ([Mo<jats:sub>3</jats:sub>S<jats:sub>13</jats:sub>]<jats:sup>2−</jats:sup>) for hydrogen evolution reaction (HER) or a cobalt polyoxometalate catalyst (Co<jats:sub>4</jats:sub>POM = [Co<jats:sub>4</jats:sub>(H<jats:sub>2</jats:sub>O)<jats:sub>2</jats:sub>(PW<jats:sub>9</jats:sub>O<jats:sub>34</jats:sub>)<jats:sub>2</jats:sub>]<jats:sup>10−</jats:sup>) for oxygen evolution reaction (OER). Under the optimized condition, the resulting hydrogels show catalytic activity in both cases upon visible light irradiation. In the case of OER, higher photosensitizer stability is observed compared to homogeneous systems, as the polymer environment seems to influence decomposition pathways.</jats:p>
Autoren
  • Tolga Çeper
  • Marcel Langer
  • Nikita Vashistha
  • Benjamin Dietzek‐Ivanšić
  • Carsten Streb
  • Sven Rau
  • Felix H Schacher
DOI
10.1002/marc.202300448
eISSN
1521-3927
ISSN
1022-1336
Ausgabe der Veröffentlichung
5
Zeitschrift
Macromolecular Rapid Communications
Sprache
en
Online publication date
2024
Datum der Veröffentlichung
2024
Status
Published
Herausgeber
Wiley
Herausgeber URL
http://dx.doi.org/10.1002/marc.202300448
Datum der Datenerfassung
2024
Titel
Poly(dehydroalanine)‐Based Hydrogels as Efficient Soft Matter Matrices for Light‐Driven Catalysis
Ausgabe der Zeitschrift
45

Datenquelle: Crossref

Abstract
Soft matter integration of photosensitizers and catalysts provides promising solutions to developing sustainable materials for energy conversion. Particularly, hydrogels bring unique benefits, such as spatial control and 3D-accessibility of molecular units, as well as recyclability. Herein, the preparation of polyampholyte hydrogels based on poly(dehydroalanine) (PDha) is reported. Chemically crosslinked PDha with bis-epoxy poly(ethylene glycol) leads to a transparent, self-supporting hydrogel. Due to the ionizable groups on PDha, this 3D polymeric matrix can be anionic, cationic, or zwitterionic depending on the pH value, and its high density of dynamic charges has a potential for electrostatic attachment of charged molecules. The integration of the cationic molecular photosensitizer [Ru(bpy)<sub>3</sub> ]<sup>2+</sup> (bpy = 2,2'-bipyridine) is realized, which is a reversible process controlled by pH, leading to light harvesting hydrogels. They are further combined with either a thiomolybdate catalyst ([Mo<sub>3</sub> S<sub>13</sub> ]<sup>2-</sup> ) for hydrogen evolution reaction (HER) or a cobalt polyoxometalate catalyst (Co<sub>4</sub> POM = [Co<sub>4</sub> (H<sub>2</sub> O)<sub>2</sub> (PW<sub>9</sub> O<sub>34</sub> )<sub>2</sub> ]<sup>10-</sup> ) for oxygen evolution reaction (OER). Under the optimized condition, the resulting hydrogels show catalytic activity in both cases upon visible light irradiation. In the case of OER, higher photosensitizer stability is observed compared to homogeneous systems, as the polymer environment seems to influence decomposition pathways.
Addresses
  • Institute of Organic Chemistry and Macromolecular Chemistry, Friedrich Schiller University Jena, Humboldtstraße 10, D-07743, Jena, Germany.
Autoren
  • Tolga Çeper
  • Marcel Langer
  • Nikita Vashistha
  • Benjamin Dietzek-Ivanšić
  • Carsten Streb
  • Sven Rau
  • Felix H Schacher
DOI
10.1002/marc.202300448
eISSN
1521-3927
Externe Identifier
  • PubMed Identifier: 38232973
Funding acknowledgements
  • Deutscher Akademischer Austauschdienst:
  • Deutsche Forschungsgemeinschaft: 364549901
  • The German Research Council: 364549901
Open access
false
ISSN
1022-1336
Ausgabe der Veröffentlichung
5
Zeitschrift
Macromolecular rapid communications
Schlüsselwörter
  • Alanine
  • Photosensitizing Agents
  • Hydrogels
  • Catalysis
  • Light
Sprache
eng
Medium
Print-Electronic
Online publication date
2024
Paginierung
e2300448
Datum der Veröffentlichung
2024
Status
Published
Publisher licence
CC BY
Datum der Datenerfassung
2024
Titel
Poly(dehydroalanine)-Based Hydrogels as Efficient Soft Matter Matrices for Light-Driven Catalysis.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
45

Datenquelle: Europe PubMed Central

Abstract
Soft matter integration of photosensitizers and catalysts provides promising solutions to developing sustainable materials for energy conversion. Particularly, hydrogels bring unique benefits, such as spatial control and 3D-accessibility of molecular units, as well as recyclability. Herein, the preparation of polyampholyte hydrogels based on poly(dehydroalanine) (PDha) is reported. Chemically crosslinked PDha with bis-epoxy poly(ethylene glycol) leads to a transparent, self-supporting hydrogel. Due to the ionizable groups on PDha, this 3D polymeric matrix can be anionic, cationic, or zwitterionic depending on the pH value, and its high density of dynamic charges has a potential for electrostatic attachment of charged molecules. The integration of the cationic molecular photosensitizer [Ru(bpy)3 ]2+ (bpy = 2,2'-bipyridine) is realized, which is a reversible process controlled by pH, leading to light harvesting hydrogels. They are further combined with either a thiomolybdate catalyst ([Mo3 S13 ]2- ) for hydrogen evolution reaction (HER) or a cobalt polyoxometalate catalyst (Co4 POM = [Co4 (H2 O)2 (PW9 O34 )2 ]10- ) for oxygen evolution reaction (OER). Under the optimized condition, the resulting hydrogels show catalytic activity in both cases upon visible light irradiation. In the case of OER, higher photosensitizer stability is observed compared to homogeneous systems, as the polymer environment seems to influence decomposition pathways.
Autoren
  • Tolga Çeper
  • Marcel Langer
  • Nikita Vashistha
  • Benjamin Dietzek-Ivanšić
  • Carsten Streb
  • Sven Rau
  • Felix H Schacher
Autoren-URL
https://www.ncbi.nlm.nih.gov/pubmed/38232973
DOI
10.1002/marc.202300448
eISSN
1521-3927
Funding acknowledgements
  • The German Research Council: 364549901
  • Deutscher Akademischer Austauschdienst:
  • Deutsche Forschungsgemeinschaft: 364549901
Ausgabe der Veröffentlichung
5
Zeitschrift
Macromol Rapid Commun
Schlüsselwörter
  • artificial photosynthesis
  • energy-conversion
  • hydrogen evolution reaction
  • oxygen evolution reaction
  • polyampholyte hydrogel scaffold
  • visible light-driven catalysis
  • Photosensitizing Agents
  • Hydrogels
  • Light
  • Catalysis
  • Alanine
Sprache
eng
Country
Germany
Paginierung
e2300448
Datum der Veröffentlichung
2024
Status
Published
Datum, an dem der Datensatz öffentlich gemacht wurde
2024
Titel
Poly(dehydroalanine)-Based Hydrogels as Efficient Soft Matter Matrices for Light-Driven Catalysis.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
45

Datenquelle: PubMed

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