Aqueous peptide-TiO2 interfaces: iso-energetic binding via either entropically- or enthalpically-driven mechanisms

Sultan, A., Westcott, Z., Hughes, Z.E., Palafox-Hernandez, J.P., Giesa, T., Puddu, V. ORCID: 0000-0001-5079-5508, Buehler, M.J., Perry, C.C. ORCID: 0000-0003-1517-468X and Walsh, T.R., 2016. Aqueous peptide-TiO2 interfaces: iso-energetic binding via either entropically- or enthalpically-driven mechanisms. ACS Applied Materials & Interfaces, 8, pp. 18620-18630. ISSN 1944-8244

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Abstract

A major barrier to the systematic improvement of biomimetic peptide-mediated strategies for the controlled growth of inorganic nanomaterials in environmentally benign conditions lies in the lack of clear conceptual connections between the sequence of the peptide and its surface binding affinity, with binding being facilitated by non-covalent interactions. Peptide conformation, both in the adsorbed and non-adsorbed state, is the key relationship that connects peptide-materials binding with peptide sequence. Here, we combine experimental peptide–titania binding characterization with state-of-the-art conformational sampling via molecular simulations to elucidate these structure/binding relationships for two very different titania-binding peptide sequences. The two sequences (Ti-1: QPYLFATDSLIK and Ti-2: GHTHYHAVRTQT) differ in their overall hydropathy, yet via quartz-crystal microbalance measurements and predictions from molecular simulations, we show these sequences both support very similar, strong titania-binding affinities. Our molecular simulations reveal that the two sequences exhibit profoundly different modes of surface binding, with Ti-1 acting as an entropically-driven binder while Ti-2 behaves as an enthalpically-driven binder. The integrated approach presented here provides a rational basis for peptide sequence engineering to achieve the in-situ growth and organization of titania nanostructures in aqueous media and for the design of sequences suitable for a range of technological applications that involve the interface between titania and biomolecules.

Item Type: Journal article
Publication Title: ACS Applied Materials & Interfaces
Creators: Sultan, A., Westcott, Z., Hughes, Z.E., Palafox-Hernandez, J.P., Giesa, T., Puddu, V., Buehler, M.J., Perry, C.C. and Walsh, T.R.
Publisher: American Chemical Society
Date: 29 June 2016
Volume: 8
ISSN: 1944-8244
Identifiers:
NumberType
10.1021/acsami.6b05200DOI
Divisions: Schools > School of Science and Technology
Depositing User: Linda Sullivan
Date Added: 04 Jul 2016 15:38
Last Modified: 16 Oct 2017 13:29
URI: http://irep.ntu.ac.uk/id/eprint/28069

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