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Engineering proton conductivity in melanin using metal doping

Bernard Mostert Orcid Logo, Shermiyah B. Rienecker, Margarita Sheliakina, Paul Zierep, Graeme R. Hanson, Jeffrey R. Harmer, Gerhard Schenk, Paul Meredith Orcid Logo

Journal of Materials Chemistry B, Volume: 8, Issue: 35, Pages: 8050 - 8060

Swansea University Authors: Bernard Mostert Orcid Logo, Paul Meredith Orcid Logo

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DOI (Published version): 10.1039/d0tb01390k

Abstract

Long range electrical conduction in biomaterials is an increasingly active area of research, which includes systems such as the conductive pili, proteins, biomacromolecules, biocompatible conductive polymers and their derivatives. One material of particular interest, the human skin pigment melanin,...

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Published in: Journal of Materials Chemistry B
ISSN: 2050-750X 2050-7518
Published: Royal Society of Chemistry (RSC) 2020
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URI: https://cronfa.swan.ac.uk/Record/cronfa54979
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spelling 2020-09-28T15:00:50.6974652 v2 54979 2020-08-13 Engineering proton conductivity in melanin using metal doping a353503c976a7338c7708a32e82f451f 0000-0002-9590-2124 Bernard Mostert Bernard Mostert true false 31e8fe57fa180d418afd48c3af280c2e 0000-0002-9049-7414 Paul Meredith Paul Meredith true false 2020-08-13 SPH Long range electrical conduction in biomaterials is an increasingly active area of research, which includes systems such as the conductive pili, proteins, biomacromolecules, biocompatible conductive polymers and their derivatives. One material of particular interest, the human skin pigment melanin, is a long range proton conductor and recently demonstrated as capable of proton-to-electron transduction in a solid-state electrochemical transistor platform. In this work, a novel “doping strategy” is proposed to enhance and control melanin's proton conductivity, potentially enhancing its utility as a transducing material. By chelating the transition metal ion Cu(II) into the bio-macromolecular matrix, free proton concentration and hence conductivity can be modulated. We confirm these observations by demonstrating enhanced performance in a next generation electrochemical transistor. Finally, the underlying mechanism is investigated via the use of a novel in situ hydration-controlled electron paramagnetic resonance study, deducing that the enhanced proton concentration is due to controlling the internal solid-state redox chemistry of the intrinsic polyindolequinone structure. This doping strategy should be open to any transition metal ions that bind to hydroquinone systems (e.g. polydopamine). As such, the tailoring strategy could make other soft solid-state ionic systems more accessible to applications in bioelectronics, leading to the creation of higher performance ion–electron coupled devices. Journal Article Journal of Materials Chemistry B 8 35 8050 8060 Royal Society of Chemistry (RSC) 2050-750X 2050-7518 5 8 2020 2020-08-05 10.1039/d0tb01390k COLLEGE NANME Physics COLLEGE CODE SPH Swansea University 2020-09-28T15:00:50.6974652 2020-08-13T13:19:52.5937451 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Bernard Mostert 0000-0002-9590-2124 1 Shermiyah B. Rienecker 2 Margarita Sheliakina 3 Paul Zierep 4 Graeme R. Hanson 5 Jeffrey R. Harmer 6 Gerhard Schenk 7 Paul Meredith 0000-0002-9049-7414 8 54979__18189__4706a9555a72436eb35e8c01a3563009.pdf 54979.pdf 2020-09-17T14:13:44.2822239 Output 981333 application/pdf Accepted Manuscript true 2021-08-05T00:00:00.0000000 true eng
title Engineering proton conductivity in melanin using metal doping
spellingShingle Engineering proton conductivity in melanin using metal doping
Bernard Mostert
Paul Meredith
title_short Engineering proton conductivity in melanin using metal doping
title_full Engineering proton conductivity in melanin using metal doping
title_fullStr Engineering proton conductivity in melanin using metal doping
title_full_unstemmed Engineering proton conductivity in melanin using metal doping
title_sort Engineering proton conductivity in melanin using metal doping
author_id_str_mv a353503c976a7338c7708a32e82f451f
31e8fe57fa180d418afd48c3af280c2e
author_id_fullname_str_mv a353503c976a7338c7708a32e82f451f_***_Bernard Mostert
31e8fe57fa180d418afd48c3af280c2e_***_Paul Meredith
author Bernard Mostert
Paul Meredith
author2 Bernard Mostert
Shermiyah B. Rienecker
Margarita Sheliakina
Paul Zierep
Graeme R. Hanson
Jeffrey R. Harmer
Gerhard Schenk
Paul Meredith
format Journal article
container_title Journal of Materials Chemistry B
container_volume 8
container_issue 35
container_start_page 8050
publishDate 2020
institution Swansea University
issn 2050-750X
2050-7518
doi_str_mv 10.1039/d0tb01390k
publisher Royal Society of Chemistry (RSC)
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 1
active_str 0
description Long range electrical conduction in biomaterials is an increasingly active area of research, which includes systems such as the conductive pili, proteins, biomacromolecules, biocompatible conductive polymers and their derivatives. One material of particular interest, the human skin pigment melanin, is a long range proton conductor and recently demonstrated as capable of proton-to-electron transduction in a solid-state electrochemical transistor platform. In this work, a novel “doping strategy” is proposed to enhance and control melanin's proton conductivity, potentially enhancing its utility as a transducing material. By chelating the transition metal ion Cu(II) into the bio-macromolecular matrix, free proton concentration and hence conductivity can be modulated. We confirm these observations by demonstrating enhanced performance in a next generation electrochemical transistor. Finally, the underlying mechanism is investigated via the use of a novel in situ hydration-controlled electron paramagnetic resonance study, deducing that the enhanced proton concentration is due to controlling the internal solid-state redox chemistry of the intrinsic polyindolequinone structure. This doping strategy should be open to any transition metal ions that bind to hydroquinone systems (e.g. polydopamine). As such, the tailoring strategy could make other soft solid-state ionic systems more accessible to applications in bioelectronics, leading to the creation of higher performance ion–electron coupled devices.
published_date 2020-08-05T04:08:52Z
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