Conformation and assembly of polypeptide scaffolds in templating the synthesis of silica: An example of a polylysine macromolecular "switch"

S V Patwardhan, R Maheshwari, N Mukherjee, K L Kiick, S J Clarson

Research output: Contribution to journalArticle

112 Citations (Scopus)

Abstract

Although the role of polycationic macromolecules in catalyzing the synthesis of silica structures is well established, detailed understanding of the mechanisms behind the production of silica structures of controlled morphologies remains unclear. In this study, we have used both poly-L-lysine (PLL) and/or poly-D-lysine (PDL) for silica synthesis to investigate mechanisms controlling inorganic morphologies. The formation of both spherical silica particles and hexagonal plates was observed. The formation of hexagonal plates was suggested, via circular dichroic spectroscopy (CD), to result from the assembly of helical polylysine molecules. We confirm that the formation of PLL helices is a prerequisite to the hexagonal silica synthesis. In addition, we present for the first time that the handedness of the helicity of the macromolecule does not affect the formation of hexagonal silica. We also show, by using two different silica precursors, that the precursor does not have a direct effect on the formation of hexagonal silica plates. Furthermore, when polylysine helices were converted to P-sheet structure, only silica particles were obtained, thus suggesting that the adoption of a helical conformation by PLL is required for the formation of hexagonally organized silica. These results demonstrate that the change in polylysine conformation can act as a "switch" in silica structure formation and suggest the potential for controlling morphologies and structures of inorganic materials via control of the conformation of soft macromolecular templates.

LanguageEnglish
Pages491-497
Number of pages7
JournalBiomacromolecules
Volume7
Issue number2
DOIs
Publication statusPublished - Feb 2006

Fingerprint

Polylysine
Polypeptides
Scaffolds
Silicon Dioxide
Conformations
Silica
Switches
Peptides
Lysine
Macromolecules
Spectroscopy

Keywords

  • in-vitro
  • secondary structure
  • silicification
  • biosilica
  • additives
  • peptides
  • mineralization
  • crystals
  • proteins

Cite this

Patwardhan, S V ; Maheshwari, R ; Mukherjee, N ; Kiick, K L ; Clarson, S J . / Conformation and assembly of polypeptide scaffolds in templating the synthesis of silica: An example of a polylysine macromolecular "switch". In: Biomacromolecules. 2006 ; Vol. 7, No. 2. pp. 491-497.
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Conformation and assembly of polypeptide scaffolds in templating the synthesis of silica: An example of a polylysine macromolecular "switch". / Patwardhan, S V ; Maheshwari, R ; Mukherjee, N ; Kiick, K L ; Clarson, S J .

In: Biomacromolecules, Vol. 7, No. 2, 02.2006, p. 491-497.

Research output: Contribution to journalArticle

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T1 - Conformation and assembly of polypeptide scaffolds in templating the synthesis of silica: An example of a polylysine macromolecular "switch"

AU - Patwardhan, S V

AU - Maheshwari, R

AU - Mukherjee, N

AU - Kiick, K L

AU - Clarson, S J

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AB - Although the role of polycationic macromolecules in catalyzing the synthesis of silica structures is well established, detailed understanding of the mechanisms behind the production of silica structures of controlled morphologies remains unclear. In this study, we have used both poly-L-lysine (PLL) and/or poly-D-lysine (PDL) for silica synthesis to investigate mechanisms controlling inorganic morphologies. The formation of both spherical silica particles and hexagonal plates was observed. The formation of hexagonal plates was suggested, via circular dichroic spectroscopy (CD), to result from the assembly of helical polylysine molecules. We confirm that the formation of PLL helices is a prerequisite to the hexagonal silica synthesis. In addition, we present for the first time that the handedness of the helicity of the macromolecule does not affect the formation of hexagonal silica. We also show, by using two different silica precursors, that the precursor does not have a direct effect on the formation of hexagonal silica plates. Furthermore, when polylysine helices were converted to P-sheet structure, only silica particles were obtained, thus suggesting that the adoption of a helical conformation by PLL is required for the formation of hexagonally organized silica. These results demonstrate that the change in polylysine conformation can act as a "switch" in silica structure formation and suggest the potential for controlling morphologies and structures of inorganic materials via control of the conformation of soft macromolecular templates.

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KW - additives

KW - peptides

KW - mineralization

KW - crystals

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