Biocatalytic induction of supramolecular order

Andrew R. Hirst, Sangita Roy, Meenakshi Arora, Apurba Das, Nigel Hodson, Paul Murray, Stephen Marshall, Nadeem Javid, Jan Sefcik, Job Boekhoven, Jan H. van Esch, Stefano Santabarbara, Neil T. Hunt, Rein V. Ulijn

Research output: Contribution to journalArticle

249 Citations (Scopus)

Abstract

Supramolecular gels, which demonstrate tunable functionalities, have attracted much interest in a range of areas, including healthcare, environmental protection and energy-related technologies. Preparing these materials in a reliable manner is challenging, with an increased level of kinetic defects observed at higher self-assembly rates. Here, by combining biocatalysis and molecular self-assembly, we have shown the ability to more quickly access higher-ordered structures. By simply increasing enzyme concentration, supramolecular order expressed at molecular, nano- and micro-levels is dramatically enhanced, and, importantly, the gelator concentrations remain identical. Amphiphile molecules were prepared by attaching an aromatic moiety to a dipeptide backbone capped with a methyl ester. Their self-assembly was induced by an enzyme that hydrolysed the ester. Different enzyme concentrations altered the catalytic activity and size of the enzyme clusters, affecting their mobility. This allowed structurally diverse materials that represent local minima in the free energy landscape to be accessed based on a single gelator structure.
Original languageEnglish
Pages (from-to)1089–1094
Number of pages6
JournalNature Chemistry
Volume2
Issue number12
Early online date10 Oct 2010
DOIs
Publication statusPublished - Dec 2010

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Keywords

  • sol-gel transition
  • peptide nanotubes
  • enzymatic formation
  • light-scattering
  • rational design
  • self
  • hydrogels
  • molecules
  • gelation

Cite this

Hirst, A. R., Roy, S., Arora, M., Das, A., Hodson, N., Murray, P., ... Ulijn, R. V. (2010). Biocatalytic induction of supramolecular order. Nature Chemistry, 2(12), 1089–1094. https://doi.org/10.1038/nchem.861