On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyan...
- Autores
- Ruiz, Gustavo Teodosio; Juliarena, María Paula; Ferraudi, G. J.; Lappin, A. G.; Bogges,W.; Feliz, Mario R.
- Año de publicación
- 2012
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- We have explored in this work the photo- and thermally-induced degradations of water soluble lignin in aqueous homogeneous media. Coordination complexes, Al(III) phthalocyaninetetrasulfonate ([Al III(tspc)] 3- and tspc 6- = phthalocyaninetetrasulfonate) and Co III/II dimethylglyoximate (dimethylglyoximate = DMG -) were used as catalysts of degrading processes with different mechanisms. The photodegradation was induced with visible light, λ exc ≥ 470 nm, and [Al III(tspc)] 3- as the photosensitizer of the ( 3Σ g -)O 2 to ( 1Δ g)O 2 conversion. ( 1Δ g)O 2 was the primary active species of the degrading process. [Co(DMG) 2(SO 3) 2] 3- and [Co(DMG) 2Cl 2] - in the presence and absence of SO 3 2- were used as catalysts of the thermal lignin degrading process. Differences in the mechanisms of the photo and thermally induced processes lead to some diversity of products. Adducts formed in solutions containing [Al III(tspc)] 3- and lignin have the absorption spectrum of phthalocyanine oligomers and could be located in pockets of the lignin. Under a steady state irradiation, the attack of lignin by ( 1Δ g)O 2 was followed by changes in the spectrum of the solution and by the formation of various products. The participation of O 2 ·- radicals in the mechanism photodegrading process was investigated with the pulse radiolysis technique. Different lignin radicals were produced when pulse radiolytically generated O 2 ·- and N 3 · radicals reacted with lignin. The Co III/II dimethylglyoximate catalyzed lignin degrading process was investigated in the presence and absence of SO 3 2-. Although the presence SO 3 2- in the medium is not essential, it accelerates the degrading process. This observation shows the participation of inorganic S(V) radicals, e.g., SO 3 ·-, as active species in the mechanism when SO 3 2- is present. Moreover, the pulse radiolysis experiments demonstrate that O 2 ·- can be an active species when SO 3 2- is absent.
Fil: Ruiz, Gustavo Teodosio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Juliarena, María Paula. Universidad Nacional del Centro de la Provincia de Buenos Aires. Facultad de Ciencias Exactas. Instituto de Fisica Arroyo Seco; Argentina
Fil: Ferraudi, G. J.. University of Notre Dame; Estados Unidos
Fil: Lappin, A. G.. University of Notre Dame; Estados Unidos
Fil: Bogges,W.. University of Notre Dame; Estados Unidos
Fil: Feliz, Mario R.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina - Materia
-
Al(Iii) Phthalocyaninetetrasulfonate
Catalysis
Co Iii/Ii Dimethylglyoximate
Flash Photolysis
Lignin
Pulse Radiolysis - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/81884
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oai:ri.conicet.gov.ar:11336/81884 |
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3498 |
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CONICET Digital (CONICET) |
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On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexesRuiz, Gustavo TeodosioJuliarena, María PaulaFerraudi, G. J.Lappin, A. G.Bogges,W.Feliz, Mario R.Al(Iii) PhthalocyaninetetrasulfonateCatalysisCo Iii/Ii DimethylglyoximateFlash PhotolysisLigninPulse Radiolysishttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We have explored in this work the photo- and thermally-induced degradations of water soluble lignin in aqueous homogeneous media. Coordination complexes, Al(III) phthalocyaninetetrasulfonate ([Al III(tspc)] 3- and tspc 6- = phthalocyaninetetrasulfonate) and Co III/II dimethylglyoximate (dimethylglyoximate = DMG -) were used as catalysts of degrading processes with different mechanisms. The photodegradation was induced with visible light, λ exc ≥ 470 nm, and [Al III(tspc)] 3- as the photosensitizer of the ( 3Σ g -)O 2 to ( 1Δ g)O 2 conversion. ( 1Δ g)O 2 was the primary active species of the degrading process. [Co(DMG) 2(SO 3) 2] 3- and [Co(DMG) 2Cl 2] - in the presence and absence of SO 3 2- were used as catalysts of the thermal lignin degrading process. Differences in the mechanisms of the photo and thermally induced processes lead to some diversity of products. Adducts formed in solutions containing [Al III(tspc)] 3- and lignin have the absorption spectrum of phthalocyanine oligomers and could be located in pockets of the lignin. Under a steady state irradiation, the attack of lignin by ( 1Δ g)O 2 was followed by changes in the spectrum of the solution and by the formation of various products. The participation of O 2 ·- radicals in the mechanism photodegrading process was investigated with the pulse radiolysis technique. Different lignin radicals were produced when pulse radiolytically generated O 2 ·- and N 3 · radicals reacted with lignin. The Co III/II dimethylglyoximate catalyzed lignin degrading process was investigated in the presence and absence of SO 3 2-. Although the presence SO 3 2- in the medium is not essential, it accelerates the degrading process. This observation shows the participation of inorganic S(V) radicals, e.g., SO 3 ·-, as active species in the mechanism when SO 3 2- is present. Moreover, the pulse radiolysis experiments demonstrate that O 2 ·- can be an active species when SO 3 2- is absent.Fil: Ruiz, Gustavo Teodosio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Juliarena, María Paula. Universidad Nacional del Centro de la Provincia de Buenos Aires. Facultad de Ciencias Exactas. Instituto de Fisica Arroyo Seco; ArgentinaFil: Ferraudi, G. J.. University of Notre Dame; Estados UnidosFil: Lappin, A. G.. University of Notre Dame; Estados UnidosFil: Bogges,W.. University of Notre Dame; Estados UnidosFil: Feliz, Mario R.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaPergamon-Elsevier Science Ltd2012-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/81884Ruiz, Gustavo Teodosio; Juliarena, María Paula; Ferraudi, G. J.; Lappin, A. G.; Bogges,W.; et al.; On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes; Pergamon-Elsevier Science Ltd; Polyhedron; 38; 1; 5-2012; 36-430277-5387CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0277538712000708info:eu-repo/semantics/altIdentifier/doi/10.1016/j.poly.2012.02.004info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:26:39Zoai:ri.conicet.gov.ar:11336/81884instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-15 15:26:39.631CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
title |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
spellingShingle |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes Ruiz, Gustavo Teodosio Al(Iii) Phthalocyaninetetrasulfonate Catalysis Co Iii/Ii Dimethylglyoximate Flash Photolysis Lignin Pulse Radiolysis |
title_short |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
title_full |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
title_fullStr |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
title_full_unstemmed |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
title_sort |
On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes |
dc.creator.none.fl_str_mv |
Ruiz, Gustavo Teodosio Juliarena, María Paula Ferraudi, G. J. Lappin, A. G. Bogges,W. Feliz, Mario R. |
author |
Ruiz, Gustavo Teodosio |
author_facet |
Ruiz, Gustavo Teodosio Juliarena, María Paula Ferraudi, G. J. Lappin, A. G. Bogges,W. Feliz, Mario R. |
author_role |
author |
author2 |
Juliarena, María Paula Ferraudi, G. J. Lappin, A. G. Bogges,W. Feliz, Mario R. |
author2_role |
author author author author author |
dc.subject.none.fl_str_mv |
Al(Iii) Phthalocyaninetetrasulfonate Catalysis Co Iii/Ii Dimethylglyoximate Flash Photolysis Lignin Pulse Radiolysis |
topic |
Al(Iii) Phthalocyaninetetrasulfonate Catalysis Co Iii/Ii Dimethylglyoximate Flash Photolysis Lignin Pulse Radiolysis |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
We have explored in this work the photo- and thermally-induced degradations of water soluble lignin in aqueous homogeneous media. Coordination complexes, Al(III) phthalocyaninetetrasulfonate ([Al III(tspc)] 3- and tspc 6- = phthalocyaninetetrasulfonate) and Co III/II dimethylglyoximate (dimethylglyoximate = DMG -) were used as catalysts of degrading processes with different mechanisms. The photodegradation was induced with visible light, λ exc ≥ 470 nm, and [Al III(tspc)] 3- as the photosensitizer of the ( 3Σ g -)O 2 to ( 1Δ g)O 2 conversion. ( 1Δ g)O 2 was the primary active species of the degrading process. [Co(DMG) 2(SO 3) 2] 3- and [Co(DMG) 2Cl 2] - in the presence and absence of SO 3 2- were used as catalysts of the thermal lignin degrading process. Differences in the mechanisms of the photo and thermally induced processes lead to some diversity of products. Adducts formed in solutions containing [Al III(tspc)] 3- and lignin have the absorption spectrum of phthalocyanine oligomers and could be located in pockets of the lignin. Under a steady state irradiation, the attack of lignin by ( 1Δ g)O 2 was followed by changes in the spectrum of the solution and by the formation of various products. The participation of O 2 ·- radicals in the mechanism photodegrading process was investigated with the pulse radiolysis technique. Different lignin radicals were produced when pulse radiolytically generated O 2 ·- and N 3 · radicals reacted with lignin. The Co III/II dimethylglyoximate catalyzed lignin degrading process was investigated in the presence and absence of SO 3 2-. Although the presence SO 3 2- in the medium is not essential, it accelerates the degrading process. This observation shows the participation of inorganic S(V) radicals, e.g., SO 3 ·-, as active species in the mechanism when SO 3 2- is present. Moreover, the pulse radiolysis experiments demonstrate that O 2 ·- can be an active species when SO 3 2- is absent. Fil: Ruiz, Gustavo Teodosio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina Fil: Juliarena, María Paula. Universidad Nacional del Centro de la Provincia de Buenos Aires. Facultad de Ciencias Exactas. Instituto de Fisica Arroyo Seco; Argentina Fil: Ferraudi, G. J.. University of Notre Dame; Estados Unidos Fil: Lappin, A. G.. University of Notre Dame; Estados Unidos Fil: Bogges,W.. University of Notre Dame; Estados Unidos Fil: Feliz, Mario R.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina |
description |
We have explored in this work the photo- and thermally-induced degradations of water soluble lignin in aqueous homogeneous media. Coordination complexes, Al(III) phthalocyaninetetrasulfonate ([Al III(tspc)] 3- and tspc 6- = phthalocyaninetetrasulfonate) and Co III/II dimethylglyoximate (dimethylglyoximate = DMG -) were used as catalysts of degrading processes with different mechanisms. The photodegradation was induced with visible light, λ exc ≥ 470 nm, and [Al III(tspc)] 3- as the photosensitizer of the ( 3Σ g -)O 2 to ( 1Δ g)O 2 conversion. ( 1Δ g)O 2 was the primary active species of the degrading process. [Co(DMG) 2(SO 3) 2] 3- and [Co(DMG) 2Cl 2] - in the presence and absence of SO 3 2- were used as catalysts of the thermal lignin degrading process. Differences in the mechanisms of the photo and thermally induced processes lead to some diversity of products. Adducts formed in solutions containing [Al III(tspc)] 3- and lignin have the absorption spectrum of phthalocyanine oligomers and could be located in pockets of the lignin. Under a steady state irradiation, the attack of lignin by ( 1Δ g)O 2 was followed by changes in the spectrum of the solution and by the formation of various products. The participation of O 2 ·- radicals in the mechanism photodegrading process was investigated with the pulse radiolysis technique. Different lignin radicals were produced when pulse radiolytically generated O 2 ·- and N 3 · radicals reacted with lignin. The Co III/II dimethylglyoximate catalyzed lignin degrading process was investigated in the presence and absence of SO 3 2-. Although the presence SO 3 2- in the medium is not essential, it accelerates the degrading process. This observation shows the participation of inorganic S(V) radicals, e.g., SO 3 ·-, as active species in the mechanism when SO 3 2- is present. Moreover, the pulse radiolysis experiments demonstrate that O 2 ·- can be an active species when SO 3 2- is absent. |
publishDate |
2012 |
dc.date.none.fl_str_mv |
2012-05 |
dc.type.none.fl_str_mv |
info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion http://purl.org/coar/resource_type/c_6501 info:ar-repo/semantics/articulo |
format |
article |
status_str |
publishedVersion |
dc.identifier.none.fl_str_mv |
http://hdl.handle.net/11336/81884 Ruiz, Gustavo Teodosio; Juliarena, María Paula; Ferraudi, G. J.; Lappin, A. G.; Bogges,W.; et al.; On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes; Pergamon-Elsevier Science Ltd; Polyhedron; 38; 1; 5-2012; 36-43 0277-5387 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/81884 |
identifier_str_mv |
Ruiz, Gustavo Teodosio; Juliarena, María Paula; Ferraudi, G. J.; Lappin, A. G.; Bogges,W.; et al.; On the homogeneous catalysis of the photochemical and thermal O 2-degrading of lignin in aqueous solution. Mechanistic observations on the processes catalyzed by Al III(phthalocyaninetetrasulfonate) 3- and Co III dimethylglyoximate complexes; Pergamon-Elsevier Science Ltd; Polyhedron; 38; 1; 5-2012; 36-43 0277-5387 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0277538712000708 info:eu-repo/semantics/altIdentifier/doi/10.1016/j.poly.2012.02.004 |
dc.rights.none.fl_str_mv |
info:eu-repo/semantics/openAccess https://creativecommons.org/licenses/by-nc-nd/2.5/ar/ |
eu_rights_str_mv |
openAccess |
rights_invalid_str_mv |
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/ |
dc.format.none.fl_str_mv |
application/pdf application/pdf application/pdf application/pdf |
dc.publisher.none.fl_str_mv |
Pergamon-Elsevier Science Ltd |
publisher.none.fl_str_mv |
Pergamon-Elsevier Science Ltd |
dc.source.none.fl_str_mv |
reponame:CONICET Digital (CONICET) instname:Consejo Nacional de Investigaciones Científicas y Técnicas |
reponame_str |
CONICET Digital (CONICET) |
collection |
CONICET Digital (CONICET) |
instname_str |
Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.name.fl_str_mv |
CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.mail.fl_str_mv |
dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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1846083409383784448 |
score |
13.22299 |