Biocatalytic self-assembly on magnetic nanoparticles

Maria P. Conte, Jugal Kishore Sahoo, Yousef M. Abul-Haija, K. H. Aaron Lau, Rein V. Ulijn

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

Combining (bio-)catalysis and molecular self-assembly provides an effective approach for the production and processing of self-assembled materials, by exploiting catalysis to direct the assembly kinetics and hence control the formation of ordered nanostructures. Applications of (bio-)catalytic self-assembly in biologically interfacing systems and in nanofabrication have recently been reported. Inspired by self-assembly in biological cells, efforts to confine catalysts on flat or patterned surfaces to exert spatial control over molecular gelator generation and nanostructure self-assembly have also emerged. Building on our previous work in the area, we demonstrate in this report the use of enzymes immobilized onto magnetic nanoparticles (NPs) to spatially localize the initiation of peptide self-assembly into nanofibers around NPs. The concept is generalized for both an equilibrium biocatalytic system that forms stable hydrogels and a non-equilibrium system that normally has a preset lifetime. Characterization of the hydrogels shows that self-assembly occurs at the site of enzyme immobilization on the NPs, to give rise to gels with a “hub-and-spoke” morphology where the nanofibers are linked through the enzyme-NP conjugates. This NP-controlled arrangement of self-assembled nanofibers enables remarkable enhancements in the shear strength of both hydrogel systems, as well as a dramatic extension of the hydrogel stability in the non-equilibrium system. We are also able to show that the use of magnetic NPs enables external control of both the formation of the hydrogel and its overall structure by application of an external magnetic field. We anticipate that the enhanced properties and stimuli-responsiveness of our NP-enzyme system will have applications ranging from nanomaterial fabrication to biomaterials and biosensing.
LanguageEnglish
Pages3069-3075
Number of pages7
JournalACS Applied Materials and Interfaces
Volume10
Issue number3
Early online date28 Dec 2017
DOIs
Publication statusPublished - 24 Jan 2018

Fingerprint

Self assembly
Hydrogels
Nanoparticles
Hydrogel
Nanofibers
Enzymes
Nanostructures
Enzyme immobilization
Immobilized Enzymes
Biocompatible Materials
Nanotechnology
Nanostructured materials
Biomaterials
Shear strength
Peptides
Catalysis
Gels
Magnetic fields
Fabrication
Catalysts

Keywords

  • biocatalysis
  • enzyme immobilization
  • magnetic nanoparticles
  • peptides
  • self-assembly

Cite this

Conte, Maria P. ; Sahoo, Jugal Kishore ; Abul-Haija, Yousef M. ; Lau, K. H. Aaron ; Ulijn, Rein V. / Biocatalytic self-assembly on magnetic nanoparticles. In: ACS Applied Materials and Interfaces. 2018 ; Vol. 10, No. 3. pp. 3069-3075.
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Biocatalytic self-assembly on magnetic nanoparticles. / Conte, Maria P.; Sahoo, Jugal Kishore; Abul-Haija, Yousef M.; Lau, K. H. Aaron; Ulijn, Rein V.

In: ACS Applied Materials and Interfaces, Vol. 10, No. 3, 24.01.2018, p. 3069-3075.

Research output: Contribution to journalArticle

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T1 - Biocatalytic self-assembly on magnetic nanoparticles

AU - Conte, Maria P.

AU - Sahoo, Jugal Kishore

AU - Abul-Haija, Yousef M.

AU - Lau, K. H. Aaron

AU - Ulijn, Rein V.

PY - 2018/1/24

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AB - Combining (bio-)catalysis and molecular self-assembly provides an effective approach for the production and processing of self-assembled materials, by exploiting catalysis to direct the assembly kinetics and hence control the formation of ordered nanostructures. Applications of (bio-)catalytic self-assembly in biologically interfacing systems and in nanofabrication have recently been reported. Inspired by self-assembly in biological cells, efforts to confine catalysts on flat or patterned surfaces to exert spatial control over molecular gelator generation and nanostructure self-assembly have also emerged. Building on our previous work in the area, we demonstrate in this report the use of enzymes immobilized onto magnetic nanoparticles (NPs) to spatially localize the initiation of peptide self-assembly into nanofibers around NPs. The concept is generalized for both an equilibrium biocatalytic system that forms stable hydrogels and a non-equilibrium system that normally has a preset lifetime. Characterization of the hydrogels shows that self-assembly occurs at the site of enzyme immobilization on the NPs, to give rise to gels with a “hub-and-spoke” morphology where the nanofibers are linked through the enzyme-NP conjugates. This NP-controlled arrangement of self-assembled nanofibers enables remarkable enhancements in the shear strength of both hydrogel systems, as well as a dramatic extension of the hydrogel stability in the non-equilibrium system. We are also able to show that the use of magnetic NPs enables external control of both the formation of the hydrogel and its overall structure by application of an external magnetic field. We anticipate that the enhanced properties and stimuli-responsiveness of our NP-enzyme system will have applications ranging from nanomaterial fabrication to biomaterials and biosensing.

KW - biocatalysis

KW - enzyme immobilization

KW - magnetic nanoparticles

KW - peptides

KW - self-assembly

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DO - 10.1021/acsami.7b15456

M3 - Article

VL - 10

SP - 3069

EP - 3075

JO - ACS Applied Materials and Interfaces

T2 - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

SN - 1944-8244

IS - 3

ER -