Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release

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 tra...

Descripción completa

Guardado en:
Detalles Bibliográficos
Autores principales: Wang, Changlong, Tuninetti, Jimena Soledad, Wang, Zhao, Zhang, Chen, Ciganda, Roberto, Salmon, Lionel, Moya, Sergio, Ruiz, Jaime, Astruc, Didier
Formato: Articulo Preprint
Lenguaje:Inglés
Publicado: 2017
Materias:
Química
Catalysis
Zif-8
Acceso en línea:http://sedici.unlp.edu.ar/handle/10915/101971
https://ri.conicet.gov.ar/11336/64286
Aporte de:
SEDICI (UNLP) de Universidad Nacional de La Plata
id I19-R120-10915-101971
record_format dspace
institution Universidad Nacional de La Plata
institution_str I-19
repository_str R-120
collection SEDICI (UNLP)
language Inglés
topic Química
Catalysis
Zif-8
spellingShingle Química
Catalysis
Zif-8
Wang, Changlong
Tuninetti, Jimena Soledad
Wang, Zhao
Zhang, Chen
Ciganda, Roberto
Salmon, Lionel
Moya, Sergio
Ruiz, Jaime
Astruc, Didier
Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release
topic_facet Química
Catalysis
Zif-8
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.
format Articulo
Preprint
author Wang, Changlong
Tuninetti, Jimena Soledad
Wang, Zhao
Zhang, Chen
Ciganda, Roberto
Salmon, Lionel
Moya, Sergio
Ruiz, Jaime
Astruc, Didier
author_facet Wang, Changlong
Tuninetti, Jimena Soledad
Wang, Zhao
Zhang, Chen
Ciganda, Roberto
Salmon, Lionel
Moya, Sergio
Ruiz, Jaime
Astruc, Didier
author_sort Wang, Changlong
title Hydrolysis of Ammonia-Borane over Ni/ZIF-8 Nanocatalyst: High Efficiency, Mechanism, and Controlled Hydrogen Release
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
publishDate 2017
url http://sedici.unlp.edu.ar/handle/10915/101971
https://ri.conicet.gov.ar/11336/64286
work_keys_str_mv AT wangchanglong hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT tuninettijimenasoledad hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT wangzhao hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT zhangchen hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT cigandaroberto hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT salmonlionel hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT moyasergio hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT ruizjaime hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
AT astrucdidier hydrolysisofammoniaboraneovernizif8nanocatalysthighefficiencymechanismandcontrolledhydrogenrelease
bdutipo_str Repositorios
_version_ 1764820440635670529

Ejemplares similares