Interfacial water morphology in hydrated melanin

Martinez-Gonzalez, J. A.; Cavaye, H.; McGettrick, James; Meredith, Paul; Motovilov, K. A.; Mostert, Bernard

doi:10.1039/d1sm00777g

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Interfacial water morphology in hydrated melanin

J. A. Martinez-Gonzalez, H. Cavaye, James McGettrick

, Paul Meredith

, K. A. Motovilov, Bernard Mostert

Soft Matter, Volume: 17, Issue: 34, Pages: 7940 - 7952

Swansea University Authors: James McGettrick , Paul Meredith , Bernard Mostert

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DOI (Published version): 10.1039/d1sm00777g

Abstract

The importance of electrically functional biomaterials is increasing as researchers explore ways to utilise them in novel sensing capacities. It has been recognised that for many of these materials the state of hydration is a key parameter that can heavily affect the conductivity, particularly those...

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Published in:	Soft Matter
ISSN:	1744-683X 1744-6848
Published:	Royal Society of Chemistry (RSC) 2021
Online Access:	Check full text
URI:	https://cronfa.swan.ac.uk/Record/cronfa58097

first_indexed	2021-09-27T08:38:16Z
last_indexed	2023-01-11T14:38:27Z
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It has been recognised that for many of these materials the state of hydration is a key parameter that can heavily affect the conductivity, particularly those that rely upon ionic or proton transport as a key mechanism. However, thus far little attention has been paid to the nature of the water morphology in the hydrated state and the concomitant ionic conductivity. Presented here is an inelastic neutron scattering (INS) experiment on hydrated eumelanin, a model bioelectronic material, in order to investigate its ‘water morphology’. We develop a rigorous new methodology for performing hydration dependent INS experiments. We also model the eumelanin dry spectra with a minimalist approach whereas for higher hydration levels we are able to obtain difference spectra to extract out the water scattering signal. A key result is that the physi-sorbed water structure within eumelanin is dominated by interfacial water with the number of water layers between 3–5, and no bulk water. We also detect for the first time, the potential signatures for proton cations, most likely the Zundel ion, within a biopolymer/water system. These new signatures may be general for soft proton ionomer systems, if the systems are comprised of only interfacial water within their structure. 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M-G. acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 665593 awarded to the Science and Technology Facilities Council. J. D. McG thank the EPSRC SPECIFIC project for funding (EP/N020863/1) & WEFO (ERDF) project AIM (80708 & EP/M015254/2) for their ongoing support for XPS maintenance. P. M. is a Seˆr Cymru II National Research Chair, which is supported by the Welsh Government through the European Regional Development Fund. K. A. M. acknowledge funding from Russian Science Foundation under grant 19-73-10154. A. B. 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spelling	2022-08-16T16:44:14.7567526 v2 58097 2021-09-27 Interfacial water morphology in hydrated melanin bdbacc591e2de05180e0fd3cc13fa480 0000-0002-7719-2958 James McGettrick James McGettrick true false 31e8fe57fa180d418afd48c3af280c2e 0000-0002-9049-7414 Paul Meredith Paul Meredith true false a353503c976a7338c7708a32e82f451f 0000-0002-9590-2124 Bernard Mostert Bernard Mostert true false 2021-09-27 EAAS The importance of electrically functional biomaterials is increasing as researchers explore ways to utilise them in novel sensing capacities. It has been recognised that for many of these materials the state of hydration is a key parameter that can heavily affect the conductivity, particularly those that rely upon ionic or proton transport as a key mechanism. However, thus far little attention has been paid to the nature of the water morphology in the hydrated state and the concomitant ionic conductivity. Presented here is an inelastic neutron scattering (INS) experiment on hydrated eumelanin, a model bioelectronic material, in order to investigate its ‘water morphology’. We develop a rigorous new methodology for performing hydration dependent INS experiments. We also model the eumelanin dry spectra with a minimalist approach whereas for higher hydration levels we are able to obtain difference spectra to extract out the water scattering signal. A key result is that the physi-sorbed water structure within eumelanin is dominated by interfacial water with the number of water layers between 3–5, and no bulk water. We also detect for the first time, the potential signatures for proton cations, most likely the Zundel ion, within a biopolymer/water system. These new signatures may be general for soft proton ionomer systems, if the systems are comprised of only interfacial water within their structure. The nature of the water morphology opens up new questions about the potential ionic charge transport mechanisms within hydrated bioelectronics materials. Journal Article Soft Matter 17 34 7940 7952 Royal Society of Chemistry (RSC) 1744-683X 1744-6848 11 8 2021 2021-08-11 10.1039/d1sm00777g COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University J. A. M-G. acknowledge funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 665593 awarded to the Science and Technology Facilities Council. J. D. McG thank the EPSRC SPECIFIC project for funding (EP/N020863/1) & WEFO (ERDF) project AIM (80708 & EP/M015254/2) for their ongoing support for XPS maintenance. P. M. is a Seˆr Cymru II National Research Chair, which is supported by the Welsh Government through the European Regional Development Fund. K. A. M. acknowledge funding from Russian Science Foundation under grant 19-73-10154. A. B. M. is a Seˆr Cymru II fellow and the results incorporated in this work is supported by the Welsh Government through the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska Curie grant agreement no. 663830. 2022-08-16T16:44:14.7567526 2021-09-27T09:37:34.8174487 Faculty of Science and Engineering School of Biosciences, Geography and Physics - Physics J. A. Martinez-Gonzalez 1 H. Cavaye 2 James McGettrick 0000-0002-7719-2958 3 Paul Meredith 0000-0002-9049-7414 4 K. A. Motovilov 5 Bernard Mostert 0000-0002-9590-2124 6 58097__21035__9c7946c4edc147af9f4c08f2e1eae77a.pdf 58097.pdf 2021-09-28T15:09:02.0392941 Output 1796937 application/pdf Accepted Manuscript true 2022-08-11T00:00:00.0000000 true eng https://creativecommons.org/licenses/by-nc-nd/3.0/
title	Interfacial water morphology in hydrated melanin
spellingShingle	Interfacial water morphology in hydrated melanin James McGettrick Paul Meredith Bernard Mostert
title_short	Interfacial water morphology in hydrated melanin
title_full	Interfacial water morphology in hydrated melanin
title_fullStr	Interfacial water morphology in hydrated melanin
title_full_unstemmed	Interfacial water morphology in hydrated melanin
title_sort	Interfacial water morphology in hydrated melanin
author_id_str_mv	bdbacc591e2de05180e0fd3cc13fa480 31e8fe57fa180d418afd48c3af280c2e a353503c976a7338c7708a32e82f451f
author_id_fullname_str_mv	bdbacc591e2de05180e0fd3cc13fa480_*_James McGettrick 31e8fe57fa180d418afd48c3af280c2e__Paul Meredith a353503c976a7338c7708a32e82f451f_**_Bernard Mostert
author	James McGettrick Paul Meredith Bernard Mostert
author2	J. A. Martinez-Gonzalez H. Cavaye James McGettrick Paul Meredith K. A. Motovilov Bernard Mostert
format	Journal article
container_title	Soft Matter
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description	The importance of electrically functional biomaterials is increasing as researchers explore ways to utilise them in novel sensing capacities. It has been recognised that for many of these materials the state of hydration is a key parameter that can heavily affect the conductivity, particularly those that rely upon ionic or proton transport as a key mechanism. However, thus far little attention has been paid to the nature of the water morphology in the hydrated state and the concomitant ionic conductivity. Presented here is an inelastic neutron scattering (INS) experiment on hydrated eumelanin, a model bioelectronic material, in order to investigate its ‘water morphology’. We develop a rigorous new methodology for performing hydration dependent INS experiments. We also model the eumelanin dry spectra with a minimalist approach whereas for higher hydration levels we are able to obtain difference spectra to extract out the water scattering signal. A key result is that the physi-sorbed water structure within eumelanin is dominated by interfacial water with the number of water layers between 3–5, and no bulk water. We also detect for the first time, the potential signatures for proton cations, most likely the Zundel ion, within a biopolymer/water system. These new signatures may be general for soft proton ionomer systems, if the systems are comprised of only interfacial water within their structure. The nature of the water morphology opens up new questions about the potential ionic charge transport mechanisms within hydrated bioelectronics materials.
published_date	2021-08-11T08:05:25Z
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Interfacial water morphology in hydrated melanin

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