Shedding light on the free radical nature of sulfonated melanins
Autor(a) principal: | |
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Data de Publicação: | 2020 |
Outros Autores: | , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1021/acs.jpcb.0c08097 http://hdl.handle.net/11449/205504 |
Resumo: | Melanin, an important class of natural pigment found in the human body, has stood out as a promising bioelectronic material due to its rather unique collection of electrical properties and biocompatibility. Among the available melanin derivatives, the sulfonated form has proven to not only be able to produce homogeneous device quality thin films with excellent adhesion, even on hydrophobic surfaces, but also to act as an ion to electron transducing element. It has recently been shown that the transport physics (and dominant carrier generation) may be related to a semiquinone free radical species in these materials. Hence, a better understanding of the paramagnetic properties of sulfonated derivatives could shed light on their charge transport behavior and thus enable improvement in regard to use in bioelectronics. Motivated by this question, in this work, different sulfonated melanin derivatives were investigated by hydration-controlled, continuous-wave X-band electron paramagnetic resonance spectroscopy and electronic structure calculations. Our results show that sulfonated melanin behaves similarly to non-functionalized melanin, but demonstrates a less pronounced response to humidity vis-a-vis standard melanin. We thus speculate on the structural and charge transport behavior in light of these differences with a view to further engineering structure−property relationships. |
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Shedding light on the free radical nature of sulfonated melaninsMelanin, an important class of natural pigment found in the human body, has stood out as a promising bioelectronic material due to its rather unique collection of electrical properties and biocompatibility. Among the available melanin derivatives, the sulfonated form has proven to not only be able to produce homogeneous device quality thin films with excellent adhesion, even on hydrophobic surfaces, but also to act as an ion to electron transducing element. It has recently been shown that the transport physics (and dominant carrier generation) may be related to a semiquinone free radical species in these materials. Hence, a better understanding of the paramagnetic properties of sulfonated derivatives could shed light on their charge transport behavior and thus enable improvement in regard to use in bioelectronics. Motivated by this question, in this work, different sulfonated melanin derivatives were investigated by hydration-controlled, continuous-wave X-band electron paramagnetic resonance spectroscopy and electronic structure calculations. Our results show that sulfonated melanin behaves similarly to non-functionalized melanin, but demonstrates a less pronounced response to humidity vis-a-vis standard melanin. We thus speculate on the structural and charge transport behavior in light of these differences with a view to further engineering structure−property relationships.School of Sciences Postgraduate Program in Science and Technology of Materials (POSMAT) São Paulo State University (UNESP)São Paulo State University (UNESP)Department of Chemistry Swansea UniversityDepartment of Physics Swansea UniversitySchool of Mathematics and Physics University of QueenslandSchool of Sciences Postgraduate Program in Science and Technology of Materials (POSMAT) School of Sciences Department of Physics São Paulo State University (UNESP)School of Sciences Postgraduate Program in Science and Technology of Materials (POSMAT) São Paulo State University (UNESP)São Paulo State University (UNESP)School of Sciences Postgraduate Program in Science and Technology of Materials (POSMAT) School of Sciences Department of Physics São Paulo State University (UNESP)Universidade Estadual Paulista (Unesp)Swansea UniversityUniversity of QueenslandBatagin-Neto, A. [UNESP]Mostert, A. B.Paulin, J. V. [UNESP]Meredith, P.Graeff, C. F.O. [UNESP]2021-06-25T10:16:26Z2021-06-25T10:16:26Z2020-11-19info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article10365-10373http://dx.doi.org/10.1021/acs.jpcb.0c08097Journal of Physical Chemistry B, v. 124, n. 46, p. 10365-10373, 2020.1520-52071520-6106http://hdl.handle.net/11449/20550410.1021/acs.jpcb.0c080972-s2.0-85096456757Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengJournal of Physical Chemistry Binfo:eu-repo/semantics/openAccess2021-10-23T14:40:59Zoai:repositorio.unesp.br:11449/205504Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T23:36:38.535953Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Shedding light on the free radical nature of sulfonated melanins |
title |
Shedding light on the free radical nature of sulfonated melanins |
spellingShingle |
Shedding light on the free radical nature of sulfonated melanins Batagin-Neto, A. [UNESP] |
title_short |
Shedding light on the free radical nature of sulfonated melanins |
title_full |
Shedding light on the free radical nature of sulfonated melanins |
title_fullStr |
Shedding light on the free radical nature of sulfonated melanins |
title_full_unstemmed |
Shedding light on the free radical nature of sulfonated melanins |
title_sort |
Shedding light on the free radical nature of sulfonated melanins |
author |
Batagin-Neto, A. [UNESP] |
author_facet |
Batagin-Neto, A. [UNESP] Mostert, A. B. Paulin, J. V. [UNESP] Meredith, P. Graeff, C. F.O. [UNESP] |
author_role |
author |
author2 |
Mostert, A. B. Paulin, J. V. [UNESP] Meredith, P. Graeff, C. F.O. [UNESP] |
author2_role |
author author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (Unesp) Swansea University University of Queensland |
dc.contributor.author.fl_str_mv |
Batagin-Neto, A. [UNESP] Mostert, A. B. Paulin, J. V. [UNESP] Meredith, P. Graeff, C. F.O. [UNESP] |
description |
Melanin, an important class of natural pigment found in the human body, has stood out as a promising bioelectronic material due to its rather unique collection of electrical properties and biocompatibility. Among the available melanin derivatives, the sulfonated form has proven to not only be able to produce homogeneous device quality thin films with excellent adhesion, even on hydrophobic surfaces, but also to act as an ion to electron transducing element. It has recently been shown that the transport physics (and dominant carrier generation) may be related to a semiquinone free radical species in these materials. Hence, a better understanding of the paramagnetic properties of sulfonated derivatives could shed light on their charge transport behavior and thus enable improvement in regard to use in bioelectronics. Motivated by this question, in this work, different sulfonated melanin derivatives were investigated by hydration-controlled, continuous-wave X-band electron paramagnetic resonance spectroscopy and electronic structure calculations. Our results show that sulfonated melanin behaves similarly to non-functionalized melanin, but demonstrates a less pronounced response to humidity vis-a-vis standard melanin. We thus speculate on the structural and charge transport behavior in light of these differences with a view to further engineering structure−property relationships. |
publishDate |
2020 |
dc.date.none.fl_str_mv |
2020-11-19 2021-06-25T10:16:26Z 2021-06-25T10:16:26Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1021/acs.jpcb.0c08097 Journal of Physical Chemistry B, v. 124, n. 46, p. 10365-10373, 2020. 1520-5207 1520-6106 http://hdl.handle.net/11449/205504 10.1021/acs.jpcb.0c08097 2-s2.0-85096456757 |
url |
http://dx.doi.org/10.1021/acs.jpcb.0c08097 http://hdl.handle.net/11449/205504 |
identifier_str_mv |
Journal of Physical Chemistry B, v. 124, n. 46, p. 10365-10373, 2020. 1520-5207 1520-6106 10.1021/acs.jpcb.0c08097 2-s2.0-85096456757 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Journal of Physical Chemistry B |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
10365-10373 |
dc.source.none.fl_str_mv |
Scopus reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
_version_ |
1808129536169082880 |