Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons

Detalhes bibliográficos
Autor(a) principal: Chiavone Filho, Osvaldo
Data de Publicação: 2019
Outros Autores: Gonçalves, Ingrid A., Barauna, Jairo, Cunha Filho, Fernando José Vieira da, Vitoriano, Jussier de Oliveira, Alves Júnior, Clodomiro, Lima, Andressa Mota
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Institucional da UFRN
Texto Completo: https://repositorio.ufrn.br/handle/123456789/45049
Resumo: Reduction of silver cations followed by nanoparticle (Ag-NPs) synthesis is a model process to understand the reduction mechanism induced by a discharge over an aqueous surface, termed electrochemical plasma. This work aims at studying the silver reduction reaction steered by electrochemical plasma in the presence of other chemically active plasma-related interfaces, namely the plasma-gas and the liquid-gas interfaces. As no other plasma-induced species are able to reduce silver cations, the reduction of silver cations is employed as strategy to selectively detect the presence of hydrated electrons ( ). The results demonstrate that the global rise of pH (increase in the content of OH−), observed for discharge in the helium gas phase, occurs in connection with the silver reduction, which is interpreted as a vivid experimental evidence of the second-order recombination reaction of the (2e– aq + 2H2O → H2 + 2OH–). On the other hand, the global decrease of pH (increase in the content of H+) observed for discharge in mixed oxygenand nitrogen gas phase, is an event primarily driven by the Birkeland-Eyde process, and it is concomitant but spatially distinct from the electron injection. The acidification interferes in the NP formation, as NPs promptly dissolve in presence of HNO3. Only in complete suppression of the acidification, an experimental evidence of the reaction pathways for hydrated electron could be captured: is competitively consumed through a scavenger-like reaction (reduction of silver cations in this work) and through the second-order recombination reactions of the . The kinetic model proposed in this work further corroborates this interpretation
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spelling Chiavone Filho, OsvaldoGonçalves, Ingrid A.Barauna, JairoCunha Filho, Fernando José Vieira daVitoriano, Jussier de OliveiraAlves Júnior, ClodomiroLima, Andressa Mota2021-11-29T13:56:12Z2021-11-29T13:56:12Z2019-05AZEVEDO, I.; BARAUNA, J.; CUNHA FILHO, F. J. V.; CHIAVONE-FILHO, O.; VITORIANO, J.; ALVES-JUNIOR, C. ; LIMA, A.B. Mota. Reduction of Aqueous Ag+ Steered by Electrochemical Plasma: Connecting the Bulk pH Variation with the Reaction Pathways for Hydrated Electrons. JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY, v. 00, p. 1-14, 2019. Disponível em: https://www.scielo.br/j/jbchs/a/3SCTDyC7QczzYLzhgGmQHTD/abstract/?lang=en&format=html. Acesso em: 14 jul. 2021. https://doi.org/10.21577/0103-5053.20190020.1097-4660https://repositorio.ufrn.br/handle/123456789/4504910.21577/0103-5053.20190020Journal of Chemical Technology and BiotechnologyAttribution 3.0 Brazilhttp://creativecommons.org/licenses/by/3.0/br/info:eu-repo/semantics/openAccessAg NPs synthesisElectrochemical plasmaHydrated electronsGlow dischargeDBDJet plasmaReduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electronsinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleReduction of silver cations followed by nanoparticle (Ag-NPs) synthesis is a model process to understand the reduction mechanism induced by a discharge over an aqueous surface, termed electrochemical plasma. This work aims at studying the silver reduction reaction steered by electrochemical plasma in the presence of other chemically active plasma-related interfaces, namely the plasma-gas and the liquid-gas interfaces. As no other plasma-induced species are able to reduce silver cations, the reduction of silver cations is employed as strategy to selectively detect the presence of hydrated electrons ( ). The results demonstrate that the global rise of pH (increase in the content of OH−), observed for discharge in the helium gas phase, occurs in connection with the silver reduction, which is interpreted as a vivid experimental evidence of the second-order recombination reaction of the (2e– aq + 2H2O → H2 + 2OH–). On the other hand, the global decrease of pH (increase in the content of H+) observed for discharge in mixed oxygenand nitrogen gas phase, is an event primarily driven by the Birkeland-Eyde process, and it is concomitant but spatially distinct from the electron injection. The acidification interferes in the NP formation, as NPs promptly dissolve in presence of HNO3. Only in complete suppression of the acidification, an experimental evidence of the reaction pathways for hydrated electron could be captured: is competitively consumed through a scavenger-like reaction (reduction of silver cations in this work) and through the second-order recombination reactions of the . The kinetic model proposed in this work further corroborates this interpretationengreponame:Repositório Institucional da UFRNinstname:Universidade Federal do Rio Grande do Norte (UFRN)instacron:UFRNORIGINALReductionAqueousAg_ChivoneFilho_2019.pdfReductionAqueousAg_ChivoneFilho_2019.pdfapplication/pdf4383906https://repositorio.ufrn.br/bitstream/123456789/45049/1/ReductionAqueousAg_ChivoneFilho_2019.pdfdd0386b9ec5eb34b2ba17982eb3c7e88MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8914https://repositorio.ufrn.br/bitstream/123456789/45049/2/license_rdf4d2950bda3d176f570a9f8b328dfbbefMD52LICENSElicense.txtlicense.txttext/plain; charset=utf-81484https://repositorio.ufrn.br/bitstream/123456789/45049/3/license.txte9597aa2854d128fd968be5edc8a28d9MD53123456789/450492021-11-29 10:56:12.892oai:https://repositorio.ufrn.br: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Repositório de PublicaçõesPUBhttp://repositorio.ufrn.br/oai/opendoar:2021-11-29T13:56:12Repositório Institucional da UFRN - Universidade Federal do Rio Grande do Norte (UFRN)false
dc.title.pt_BR.fl_str_mv Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
title Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
spellingShingle Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
Chiavone Filho, Osvaldo
Ag NPs synthesis
Electrochemical plasma
Hydrated electrons
Glow discharge
DBD
Jet plasma
title_short Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
title_full Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
title_fullStr Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
title_full_unstemmed Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
title_sort Reduction of aqueous Ag+ steered by electrochemical plasma: connecting the bulk pH variation with the reaction pathways for hydrated electrons
author Chiavone Filho, Osvaldo
author_facet Chiavone Filho, Osvaldo
Gonçalves, Ingrid A.
Barauna, Jairo
Cunha Filho, Fernando José Vieira da
Vitoriano, Jussier de Oliveira
Alves Júnior, Clodomiro
Lima, Andressa Mota
author_role author
author2 Gonçalves, Ingrid A.
Barauna, Jairo
Cunha Filho, Fernando José Vieira da
Vitoriano, Jussier de Oliveira
Alves Júnior, Clodomiro
Lima, Andressa Mota
author2_role author
author
author
author
author
author
dc.contributor.author.fl_str_mv Chiavone Filho, Osvaldo
Gonçalves, Ingrid A.
Barauna, Jairo
Cunha Filho, Fernando José Vieira da
Vitoriano, Jussier de Oliveira
Alves Júnior, Clodomiro
Lima, Andressa Mota
dc.subject.por.fl_str_mv Ag NPs synthesis
Electrochemical plasma
Hydrated electrons
Glow discharge
DBD
Jet plasma
topic Ag NPs synthesis
Electrochemical plasma
Hydrated electrons
Glow discharge
DBD
Jet plasma
description Reduction of silver cations followed by nanoparticle (Ag-NPs) synthesis is a model process to understand the reduction mechanism induced by a discharge over an aqueous surface, termed electrochemical plasma. This work aims at studying the silver reduction reaction steered by electrochemical plasma in the presence of other chemically active plasma-related interfaces, namely the plasma-gas and the liquid-gas interfaces. As no other plasma-induced species are able to reduce silver cations, the reduction of silver cations is employed as strategy to selectively detect the presence of hydrated electrons ( ). The results demonstrate that the global rise of pH (increase in the content of OH−), observed for discharge in the helium gas phase, occurs in connection with the silver reduction, which is interpreted as a vivid experimental evidence of the second-order recombination reaction of the (2e– aq + 2H2O → H2 + 2OH–). On the other hand, the global decrease of pH (increase in the content of H+) observed for discharge in mixed oxygenand nitrogen gas phase, is an event primarily driven by the Birkeland-Eyde process, and it is concomitant but spatially distinct from the electron injection. The acidification interferes in the NP formation, as NPs promptly dissolve in presence of HNO3. Only in complete suppression of the acidification, an experimental evidence of the reaction pathways for hydrated electron could be captured: is competitively consumed through a scavenger-like reaction (reduction of silver cations in this work) and through the second-order recombination reactions of the . The kinetic model proposed in this work further corroborates this interpretation
publishDate 2019
dc.date.issued.fl_str_mv 2019-05
dc.date.accessioned.fl_str_mv 2021-11-29T13:56:12Z
dc.date.available.fl_str_mv 2021-11-29T13:56:12Z
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.citation.fl_str_mv AZEVEDO, I.; BARAUNA, J.; CUNHA FILHO, F. J. V.; CHIAVONE-FILHO, O.; VITORIANO, J.; ALVES-JUNIOR, C. ; LIMA, A.B. Mota. Reduction of Aqueous Ag+ Steered by Electrochemical Plasma: Connecting the Bulk pH Variation with the Reaction Pathways for Hydrated Electrons. JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY, v. 00, p. 1-14, 2019. Disponível em: https://www.scielo.br/j/jbchs/a/3SCTDyC7QczzYLzhgGmQHTD/abstract/?lang=en&format=html. Acesso em: 14 jul. 2021. https://doi.org/10.21577/0103-5053.20190020.
dc.identifier.uri.fl_str_mv https://repositorio.ufrn.br/handle/123456789/45049
dc.identifier.issn.none.fl_str_mv 1097-4660
dc.identifier.doi.none.fl_str_mv 10.21577/0103-5053.20190020
identifier_str_mv AZEVEDO, I.; BARAUNA, J.; CUNHA FILHO, F. J. V.; CHIAVONE-FILHO, O.; VITORIANO, J.; ALVES-JUNIOR, C. ; LIMA, A.B. Mota. Reduction of Aqueous Ag+ Steered by Electrochemical Plasma: Connecting the Bulk pH Variation with the Reaction Pathways for Hydrated Electrons. JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY, v. 00, p. 1-14, 2019. Disponível em: https://www.scielo.br/j/jbchs/a/3SCTDyC7QczzYLzhgGmQHTD/abstract/?lang=en&format=html. Acesso em: 14 jul. 2021. https://doi.org/10.21577/0103-5053.20190020.
1097-4660
10.21577/0103-5053.20190020
url https://repositorio.ufrn.br/handle/123456789/45049
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dc.rights.driver.fl_str_mv Attribution 3.0 Brazil
http://creativecommons.org/licenses/by/3.0/br/
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rights_invalid_str_mv Attribution 3.0 Brazil
http://creativecommons.org/licenses/by/3.0/br/
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Journal of Chemical Technology and Biotechnology
publisher.none.fl_str_mv Journal of Chemical Technology and Biotechnology
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