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

241 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.
LanguageEnglish
Pages1089–1094
Number of pages6
JournalNature Chemistry
Volume2
Issue number12
Early online date10 Oct 2010
DOIs
Publication statusPublished - Dec 2010

Fingerprint

Enzymes
Self assembly
Esters
Amphiphiles
Dipeptides
Environmental protection
Free energy
Catalyst activity
Gels
Defects
Molecules
Kinetics

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
Hirst, Andrew R. ; Roy, Sangita ; Arora, Meenakshi ; Das, Apurba ; Hodson, Nigel ; Murray, Paul ; Marshall, Stephen ; Javid, Nadeem ; Sefcik, Jan ; Boekhoven, Job ; van Esch, Jan H. ; Santabarbara, Stefano ; Hunt, Neil T. ; Ulijn, Rein V. / Biocatalytic induction of supramolecular order. In: Nature Chemistry. 2010 ; Vol. 2, No. 12. pp. 1089–1094.
@article{59215c9e77e44a2ca36fe10e8f6c0a1a,
title = "Biocatalytic induction of supramolecular order",
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.",
keywords = "sol-gel transition, peptide nanotubes, enzymatic formation, light-scattering, rational design, self, hydrogels, molecules, gelation",
author = "Hirst, {Andrew R.} and Sangita Roy and Meenakshi Arora and Apurba Das and Nigel Hodson and Paul Murray and Stephen Marshall and Nadeem Javid and Jan Sefcik and Job Boekhoven and {van Esch}, {Jan H.} and Stefano Santabarbara and Hunt, {Neil T.} and Ulijn, {Rein V.}",
year = "2010",
month = "12",
doi = "10.1038/nchem.861",
language = "English",
volume = "2",
pages = "1089–1094",
journal = "Nature Chemistry",
issn = "1755-4330",
number = "12",

}

Hirst, AR, Roy, S, Arora, M, Das, A, Hodson, N, Murray, P, Marshall, S, Javid, N, Sefcik, J, Boekhoven, J, van Esch, JH, Santabarbara, S, Hunt, NT & Ulijn, RV 2010, 'Biocatalytic induction of supramolecular order' Nature Chemistry, vol. 2, no. 12, pp. 1089–1094. https://doi.org/10.1038/nchem.861

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

In: Nature Chemistry, Vol. 2, No. 12, 12.2010, p. 1089–1094.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Biocatalytic induction of supramolecular order

AU - Hirst, Andrew R.

AU - Roy, Sangita

AU - Arora, Meenakshi

AU - Das, Apurba

AU - Hodson, Nigel

AU - Murray, Paul

AU - Marshall, Stephen

AU - Javid, Nadeem

AU - Sefcik, Jan

AU - Boekhoven, Job

AU - van Esch, Jan H.

AU - Santabarbara, Stefano

AU - Hunt, Neil T.

AU - Ulijn, Rein V.

PY - 2010/12

Y1 - 2010/12

N2 - 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.

AB - 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.

KW - sol-gel transition

KW - peptide nanotubes

KW - enzymatic formation

KW - light-scattering

KW - rational design

KW - self

KW - hydrogels

KW - molecules

KW - gelation

UR - http://www.nature.com/nchem/journal/v2/n12/full/nchem.861.html

U2 - 10.1038/nchem.861

DO - 10.1038/nchem.861

M3 - Article

VL - 2

SP - 1089

EP - 1094

JO - Nature Chemistry

T2 - Nature Chemistry

JF - Nature Chemistry

SN - 1755-4330

IS - 12

ER -

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