Encapsulating [FeFe]-hydrogenase model compounds in peptide hydrogels dramatically modifies stability and photochemistry

Pim Frederix, Rafal Kania, Joseph A. Wright, Dimitrios Lamprou, Rein Ulijn, Christopher J. Pickett, Neil Hunt

Research output: Contribution to journalArticle

25 Citations (Scopus)

Abstract

A [FeFe]-hydrogenase model compound (µ-S(CH2)3S)Fe2(CO)4(PMe3)2 [1] has been encapsulated in a Low Molecular Weight (LMW) hydrogelator (Fmoc-Leu-Leu). Linear infrared absorption spectroscopy, gel melting and ultrafast time-resolved infrared spectroscopy experiments reveal significant contrasts in chemical environment and photochemistry between the encapsulated molecules and solution phase systems. Specifically, the gel provides a more rigid hydrogen bonding environment, which restricts isomerisation following photolysis while imparting significant increases in stability relative to a similarly aqueous solution. Since understanding and ultimately controlling the mechanistic role of ligands near Fe centers is likely to be crucial in exploiting artificial hydrogenases, these gels may offer a new option for future materials design involving catalysts.


Original languageEnglish
Pages (from-to)13112-13119
Number of pages8
JournalDalton Transactions
Volume41
Issue number42
Early online date28 Mar 2012
DOIs
Publication statusPublished - 12 Oct 2012

Fingerprint

Hydrogenase
Hydrogels
Photochemical reactions
Gels
Peptides
Infrared spectroscopy
Photolysis
Infrared absorption
Carbon Monoxide
Isomerization
Absorption spectroscopy
Hydrogen bonds
Melting
Molecular weight
Ligands
Catalysts
Molecules
Experiments

Keywords

  • [FeFe]-hydrogenase model compound
  • peptide hydrogels
  • stability
  • photochemistry
  • chemical environment
  • encapsulated molecules
  • solution phase systems
  • artificial hydrogenases

Cite this

Frederix, Pim ; Kania, Rafal ; Wright, Joseph A. ; Lamprou, Dimitrios ; Ulijn, Rein ; Pickett, Christopher J. ; Hunt, Neil. / Encapsulating [FeFe]-hydrogenase model compounds in peptide hydrogels dramatically modifies stability and photochemistry. In: Dalton Transactions. 2012 ; Vol. 41, No. 42. pp. 13112-13119.
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Encapsulating [FeFe]-hydrogenase model compounds in peptide hydrogels dramatically modifies stability and photochemistry. / Frederix, Pim; Kania, Rafal; Wright, Joseph A.; Lamprou, Dimitrios; Ulijn, Rein; Pickett, Christopher J.; Hunt, Neil.

In: Dalton Transactions, Vol. 41, No. 42, 12.10.2012, p. 13112-13119.

Research output: Contribution to journalArticle

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