Force field and a surface model database for silica to simulate interfacial properties in atomic resolution

Fateme S. Emami, Valeria Puddu, Rajiv J. Berry, Vikas Varshney, Siddharth Patwardhan, Carole C. Perry, Hendrik Heinz

Research output: Contribution to journalArticle

136 Citations (Scopus)

Abstract

Silica nanostructures find applications in drug delivery, catalysis, and composites, however, understanding of the surface chemistry, aqueous interfaces, and biomolecule recognition remain difficult using current imaging techniques and spectroscopy. A silica force field is introduced that resolves numerous shortcomings of prior silica force fields over the last 30 years and reduces uncertainties in computed interfacial properties relative to experiment from several 100% to less than 5%. In addition, a silica surface model database is introduced for the full range of variable surface chemistry and pH (Q2, Q3, Q4 environments with adjustable degree of ionization) that have shown to determine selective molecular recognition. The force field enables accurate computational predictions of aqueous interfacial properties of all types of silica, which is substantiated by extensive comparisons to experimental measurements. The parameters are integrated into multiple force fields for broad applicability to biomolecules, polymers, and inorganic materials (AMBER, CHARMM, COMPASS, CVFF, PCFF, INTERFACE force fields). We also explain mechanistic details of molecular adsorption of water vapor, as well as significant variations in the amount and dissociation depth of superficial cations at silica–water interfaces that correlate with ζ-potential measurements and create a wide range of aqueous environments for adsorption and self-assembly of complex molecules. The systematic analysis of binding conformations and adsorption free energies of distinct peptides to silica surfaces will be reported separately in a companion paper. The models aid to understand and design silica nanomaterials in 3D atomic resolution and are extendable to chemical reactions.
LanguageEnglish
Pages2647–2658
Number of pages12
JournalChemistry of Materials
Volume26
Issue number8
Early online date18 Mar 2014
DOIs
Publication statusPublished - 22 Apr 2014

Fingerprint

Silicon Dioxide
Silica
Biomolecules
Surface chemistry
Adsorption
Amber
Molecular recognition
Steam
Zeta potential
Drug delivery
Nanostructured materials
Self assembly
Water vapor
Peptides
Catalysis
Free energy
Ionization
Conformations
Cations
Chemical reactions

Keywords

  • silica nanostructures
  • drug delivery
  • surface chemistry
  • aqueous interfaces
  • biomolecule recognition
  • water vapor

Cite this

Emami, F. S., Puddu, V., Berry, R. J., Varshney, V., Patwardhan, S., Perry, C. C., & Heinz, H. (2014). Force field and a surface model database for silica to simulate interfacial properties in atomic resolution. Chemistry of Materials, 26(8), 2647–2658. https://doi.org/10.1021/cm500365c
Emami, Fateme S. ; Puddu, Valeria ; Berry, Rajiv J. ; Varshney, Vikas ; Patwardhan, Siddharth ; Perry, Carole C. ; Heinz, Hendrik. / Force field and a surface model database for silica to simulate interfacial properties in atomic resolution. In: Chemistry of Materials. 2014 ; Vol. 26, No. 8. pp. 2647–2658.
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Emami, FS, Puddu, V, Berry, RJ, Varshney, V, Patwardhan, S, Perry, CC & Heinz, H 2014, 'Force field and a surface model database for silica to simulate interfacial properties in atomic resolution' Chemistry of Materials, vol. 26, no. 8, pp. 2647–2658. https://doi.org/10.1021/cm500365c

Force field and a surface model database for silica to simulate interfacial properties in atomic resolution. / Emami, Fateme S.; Puddu, Valeria; Berry, Rajiv J.; Varshney, Vikas; Patwardhan, Siddharth; Perry, Carole C.; Heinz, Hendrik.

In: Chemistry of Materials, Vol. 26, No. 8, 22.04.2014, p. 2647–2658.

Research output: Contribution to journalArticle

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T1 - Force field and a surface model database for silica to simulate interfacial properties in atomic resolution

AU - Emami, Fateme S.

AU - Puddu, Valeria

AU - Berry, Rajiv J.

AU - Varshney, Vikas

AU - Patwardhan, Siddharth

AU - Perry, Carole C.

AU - Heinz, Hendrik

PY - 2014/4/22

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AB - Silica nanostructures find applications in drug delivery, catalysis, and composites, however, understanding of the surface chemistry, aqueous interfaces, and biomolecule recognition remain difficult using current imaging techniques and spectroscopy. A silica force field is introduced that resolves numerous shortcomings of prior silica force fields over the last 30 years and reduces uncertainties in computed interfacial properties relative to experiment from several 100% to less than 5%. In addition, a silica surface model database is introduced for the full range of variable surface chemistry and pH (Q2, Q3, Q4 environments with adjustable degree of ionization) that have shown to determine selective molecular recognition. The force field enables accurate computational predictions of aqueous interfacial properties of all types of silica, which is substantiated by extensive comparisons to experimental measurements. The parameters are integrated into multiple force fields for broad applicability to biomolecules, polymers, and inorganic materials (AMBER, CHARMM, COMPASS, CVFF, PCFF, INTERFACE force fields). We also explain mechanistic details of molecular adsorption of water vapor, as well as significant variations in the amount and dissociation depth of superficial cations at silica–water interfaces that correlate with ζ-potential measurements and create a wide range of aqueous environments for adsorption and self-assembly of complex molecules. The systematic analysis of binding conformations and adsorption free energies of distinct peptides to silica surfaces will be reported separately in a companion paper. The models aid to understand and design silica nanomaterials in 3D atomic resolution and are extendable to chemical reactions.

KW - silica nanostructures

KW - drug delivery

KW - surface chemistry

KW - aqueous interfaces

KW - biomolecule recognition

KW - water vapor

UR - http://pubs.acs.org/doi/abs/10.1021/cm500365c

U2 - 10.1021/cm500365c

DO - 10.1021/cm500365c

M3 - Article

VL - 26

SP - 2647

EP - 2658

JO - Chemistry of Materials

T2 - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 8

ER -