Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release
- Autores
- Wang, Changlong; Tuninetti, Jimena Soledad; Wang, Zhao; Zhang, Chen; Ciganda, Roberto; Salmon, Lionel; Moya, Sergio; Ruiz, Jaime; Astruc, Didier
- Año de publicación
- 2017
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- Non-noble metal nanoparticles are notoriously difficult to prepare and stabilize with appropriate dispersion, which in turn severely limits their catalytic functions. Here, using zeolitic imidazolate framework (ZIF-8) as MOF template, catalytically remarkably efficient ligand-free first-row late transition-metal nanoparticles are prepared and compared. Upon scrutiny of the catalytic principles in the hydrolysis of ammonia-borane, the highest total turnover frequency among these first-row late transition metals is achieved for the templated Ni nanoparticles with 85.7 molH2 molcat -1 min-1 at room temperature, which overtakes performances of previous non-noble metal nanoparticles systems, and is even better than some noble metal nanoparticles systems. Mechanistic studies especially using kinetic isotope effects show that cleavage by oxidative addition of an O-H bond in H2O is the rate-determining step in this reaction. Inspired by these mechanistic studies, an attractive and effective "on-off" control of hydrogen production is further proposed.
Fil: Wang, Changlong. Centre National de la Recherche Scientifique/laboratoir; Francia
Fil: Tuninetti, Jimena Soledad. 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: Wang, Zhao. Sorbonne Universités; Francia
Fil: Zhang, Chen. Sorbonne Universites; Francia
Fil: Ciganda, Roberto. Universite Bordeaux; Francia
Fil: Salmon, Lionel. Laboratoire de Chimie de Coordination; Francia
Fil: Moya, Sergio. Cic Biomagune; España
Fil: Ruiz, Jaime. Universite de Bordeaux; Francia
Fil: Astruc, Didier. Universite de Bordeaux; Francia - Materia
-
CATALYSIS
ZIF-8 - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
- Repositorio
.jpg)
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/64286
Ver los metadatos del registro completo
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Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen ReleaseWang, ChanglongTuninetti, Jimena SoledadWang, ZhaoZhang, ChenCiganda, RobertoSalmon, LionelMoya, SergioRuiz, JaimeAstruc, DidierCATALYSISZIF-8https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Non-noble metal nanoparticles are notoriously difficult to prepare and stabilize with appropriate dispersion, which in turn severely limits their catalytic functions. Here, using zeolitic imidazolate framework (ZIF-8) as MOF template, catalytically remarkably efficient ligand-free first-row late transition-metal nanoparticles are prepared and compared. Upon scrutiny of the catalytic principles in the hydrolysis of ammonia-borane, the highest total turnover frequency among these first-row late transition metals is achieved for the templated Ni nanoparticles with 85.7 molH2 molcat -1 min-1 at room temperature, which overtakes performances of previous non-noble metal nanoparticles systems, and is even better than some noble metal nanoparticles systems. Mechanistic studies especially using kinetic isotope effects show that cleavage by oxidative addition of an O-H bond in H2O is the rate-determining step in this reaction. Inspired by these mechanistic studies, an attractive and effective "on-off" control of hydrogen production is further proposed.Fil: Wang, Changlong. Centre National de la Recherche Scientifique/laboratoir; FranciaFil: Tuninetti, Jimena Soledad. 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: Wang, Zhao. Sorbonne Universités; FranciaFil: Zhang, Chen. Sorbonne Universites; FranciaFil: Ciganda, Roberto. Universite Bordeaux; FranciaFil: Salmon, Lionel. Laboratoire de Chimie de Coordination; FranciaFil: Moya, Sergio. Cic Biomagune; EspañaFil: Ruiz, Jaime. Universite de Bordeaux; FranciaFil: Astruc, Didier. Universite de Bordeaux; FranciaAmerican Chemical Society2017-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/64286Wang, Changlong; Tuninetti, Jimena Soledad; Wang, Zhao; Zhang, Chen; Ciganda, Roberto; et al.; Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release; American Chemical Society; Journal of the American Chemical Society; 139; 33; 8-2017; 11610-116150002-7863CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jacs.7b06859info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.7b06859info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-11-12T09:49:53Zoai:ri.conicet.gov.ar:11336/64286instacron: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:34982025-11-12 09:49:53.583CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
| dc.title.none.fl_str_mv |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| title |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| spellingShingle |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release Wang, Changlong CATALYSIS ZIF-8 |
| title_short |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| title_full |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| title_fullStr |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| title_full_unstemmed |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| title_sort |
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release |
| dc.creator.none.fl_str_mv |
Wang, Changlong Tuninetti, Jimena Soledad Wang, Zhao Zhang, Chen Ciganda, Roberto Salmon, Lionel Moya, Sergio Ruiz, Jaime Astruc, Didier |
| author |
Wang, Changlong |
| author_facet |
Wang, Changlong Tuninetti, Jimena Soledad Wang, Zhao Zhang, Chen Ciganda, Roberto Salmon, Lionel Moya, Sergio Ruiz, Jaime Astruc, Didier |
| author_role |
author |
| author2 |
Tuninetti, Jimena Soledad Wang, Zhao Zhang, Chen Ciganda, Roberto Salmon, Lionel Moya, Sergio Ruiz, Jaime Astruc, Didier |
| author2_role |
author author author author author author author author |
| dc.subject.none.fl_str_mv |
CATALYSIS ZIF-8 |
| topic |
CATALYSIS ZIF-8 |
| purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
| dc.description.none.fl_txt_mv |
Non-noble metal nanoparticles are notoriously difficult to prepare and stabilize with appropriate dispersion, which in turn severely limits their catalytic functions. Here, using zeolitic imidazolate framework (ZIF-8) as MOF template, catalytically remarkably efficient ligand-free first-row late transition-metal nanoparticles are prepared and compared. Upon scrutiny of the catalytic principles in the hydrolysis of ammonia-borane, the highest total turnover frequency among these first-row late transition metals is achieved for the templated Ni nanoparticles with 85.7 molH2 molcat -1 min-1 at room temperature, which overtakes performances of previous non-noble metal nanoparticles systems, and is even better than some noble metal nanoparticles systems. Mechanistic studies especially using kinetic isotope effects show that cleavage by oxidative addition of an O-H bond in H2O is the rate-determining step in this reaction. Inspired by these mechanistic studies, an attractive and effective "on-off" control of hydrogen production is further proposed. Fil: Wang, Changlong. Centre National de la Recherche Scientifique/laboratoir; Francia Fil: Tuninetti, Jimena Soledad. 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: Wang, Zhao. Sorbonne Universités; Francia Fil: Zhang, Chen. Sorbonne Universites; Francia Fil: Ciganda, Roberto. Universite Bordeaux; Francia Fil: Salmon, Lionel. Laboratoire de Chimie de Coordination; Francia Fil: Moya, Sergio. Cic Biomagune; España Fil: Ruiz, Jaime. Universite de Bordeaux; Francia Fil: Astruc, Didier. Universite de Bordeaux; Francia |
| description |
Non-noble metal nanoparticles are notoriously difficult to prepare and stabilize with appropriate dispersion, which in turn severely limits their catalytic functions. Here, using zeolitic imidazolate framework (ZIF-8) as MOF template, catalytically remarkably efficient ligand-free first-row late transition-metal nanoparticles are prepared and compared. Upon scrutiny of the catalytic principles in the hydrolysis of ammonia-borane, the highest total turnover frequency among these first-row late transition metals is achieved for the templated Ni nanoparticles with 85.7 molH2 molcat -1 min-1 at room temperature, which overtakes performances of previous non-noble metal nanoparticles systems, and is even better than some noble metal nanoparticles systems. Mechanistic studies especially using kinetic isotope effects show that cleavage by oxidative addition of an O-H bond in H2O is the rate-determining step in this reaction. Inspired by these mechanistic studies, an attractive and effective "on-off" control of hydrogen production is further proposed. |
| publishDate |
2017 |
| dc.date.none.fl_str_mv |
2017-08 |
| 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/11336/64286 Wang, Changlong; Tuninetti, Jimena Soledad; Wang, Zhao; Zhang, Chen; Ciganda, Roberto; et al.; Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release; American Chemical Society; Journal of the American Chemical Society; 139; 33; 8-2017; 11610-11615 0002-7863 CONICET Digital CONICET |
| url |
http://hdl.handle.net/11336/64286 |
| identifier_str_mv |
Wang, Changlong; Tuninetti, Jimena Soledad; Wang, Zhao; Zhang, Chen; Ciganda, Roberto; et al.; Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release; American Chemical Society; Journal of the American Chemical Society; 139; 33; 8-2017; 11610-11615 0002-7863 CONICET Digital CONICET |
| dc.language.none.fl_str_mv |
eng |
| language |
eng |
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info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jacs.7b06859 info:eu-repo/semantics/altIdentifier/doi/10.1021/jacs.7b06859 |
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info:eu-repo/semantics/openAccess https://creativecommons.org/licenses/by-nc-sa/2.5/ar/ |
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openAccess |
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https://creativecommons.org/licenses/by-nc-sa/2.5/ar/ |
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application/pdf application/pdf |
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American Chemical Society |
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American Chemical Society |
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Consejo Nacional de Investigaciones Científicas y Técnicas |
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CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
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dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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