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Theoretical Study of Size Effects on Surface Chemical Properties for Nanoscale Diamond Particles
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
2014 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 118, no 45, 26061-26069 p.Article in journal (Refereed) Published
Abstract [en]

Nanodiamond has displayed some unique physical and chemical properties compared to bulk diamond, which broadens its applications in various areas. However, a more detailed picture of nanodiamond quantum confinements is still missing from a theoretical point of view. This investigation presents a study where the effects of one-dimension (i.e., diamond thin films) and three-dimension (i.e., nanodiamond particles) confinement on surface reactivity, and properties, have been calculated using density functional theory (DFT) and tight binding density functional theory (DFTB) methods. Surface specific parameters like (i) surface C–H bond length, (ii) atomic charges, (iii) H adsorption energy, (iv) highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO), (v) band gap, and (vi) Fukui functions were thereby carefully calculated and compared. For both the one-dimensional diamond thin films of different surface planes, quantum confinements have strong influences on these factors from thickness of 0.2 to ∼1 nm, while for thin films thicker than 1 nm, the values stabilize around a plateau value. For three-dimensional situations, these factors were found to change within a range of nanodiamond diameter of 0.4 to ∼2 nm, followed by oscillations around specific values as well. These results reveal that nanoscale diamond quantum confinements exist for a nanodiamond particle of a diameter smaller than 2 nm, but not for larger particle sizes. It must here be stressed that all surface specific parameters did independently show the existence of the here presented size ranges for quantum confinement.

Place, publisher, year, edition, pages
Washington, D.C.: American Chemical Society (ACS), 2014. Vol. 118, no 45, 26061-26069 p.
Keyword [en]
Nano-scale diamond, DFTB, Nanodiamond
National Category
Nano Technology
Research subject
Chemistry with specialization in Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-236449DOI: 10.1021/jp507421uISI: 000344978000029OAI: oai:DiVA.org:uu-236449DiVA: diva2:764502
Projects
Vascubone
Funder
EU, FP7, Seventh Framework Programme, 242175
Available from: 2014-11-19 Created: 2014-11-19 Last updated: 2017-12-05Bibliographically approved
In thesis
1. Biomolecule Functionalization of Diamond Surfaces for Implant Applications - A Theoretical Study
Open this publication in new window or tab >>Biomolecule Functionalization of Diamond Surfaces for Implant Applications - A Theoretical Study
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Diamond is a promising material with unique chemical properties. In this thesis, nano-scale diamond quantum size effects were investigated using several chemical property indicators. The results show that the chemical properties are strongly dependent on size for film thicknesses smaller than 1 nm (1D), and for nanodiamond particle diameters less than 2 nm (3D). When the sizes exceed these ranges there are no longer any quantum effects.

The influence of surface termination coverage on the surface chemical properties has been calculated for the 2×1 reconstructed diamond (100) surface and for the diamond (111) surface. The terminating species included COOH and NH2 groups, which both are beneficial for the immobilization of biomolecules. The results of the calculations show that it is energetically possible to terminate the diamond surfaces up to 100% with NH2, while it is only possible to cover the surfaces up to 50% with COOH species. The reason for the latter result is most probably the larger sterical hindrance amongst the adsorbates. Both types of termination species were shown to influence the diamond surface electronic properties (e.g., HOMO/LUMO levels).

In order to extend the diamond utility for biomedical applications, especially implant design, interactions of various growth factors with the diamond surfaces were also simulated. For non-solvent diamond-biomolecule systems, the results show that adhesion affinities are strongly dependent on biomolecule molecular weights. When including a water based solvent in the systems, the results show good physisorption affinities between proteins and diamond. Proteins structures, before and after physisorption, were visualized, and further investigated with respect to electrostatic properties and functional groups. By comparing the biomolecular structural changes during the adhesion processes, it can be concluded that both the general structures, as well as the binding pocket structures, were kept intact after the adhesion to the diamond surfaces (regardless of the adhesion affinities). In addition, the surface electronic potential distributions were maintained, which indicate preserved biomolecule functionalities.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2015. 79 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1210
Keyword
Diamond, Biomolecules, Functionalization, VEGF, BMP2, Fibronectin, Chitosan, Heparin, RGD peptide, Angiopoietin, Theoretical
National Category
Medical Materials Theoretical Chemistry
Research subject
Chemistry with specialization in Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-236957 (URN)978-91-554-9118-5 (ISBN)
Public defence
2015-01-28, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
Opponent
Supervisors
Projects
Vascubone
Available from: 2015-01-07 Created: 2014-11-25 Last updated: 2015-02-03

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Publisher's full texthttp://pubs.acs.org/doi/abs/10.1021/jp507421u

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Tian, YuanLarsson, Karin

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