Synergetic Effect of Ultrasmall Metal Clusters and Zeolites Promoting Hydrogen Generation
Open Access
- 25 March 2019
- journal article
- research article
- Published by Wiley in Advanced Science
- Vol. 6 (10), 1802350
- https://doi.org/10.1002/advs.201802350
Abstract
Taking advantage of the synergetic effect of confined ultrasmall metal clusters and zeolite frameworks is an efficient strategy for improving the catalytic performance of metal nanocatalysts. Herein, it is demonstrated that the synergetic effect of ultrasmall ruthenium (Ru) clusters and intrinsic Brønsted acidity of zeolite frameworks can significantly promote the hydrogen generation of ammonia borane (AB) hydrolysis. Ultrasmall Ru clusters are embedded onto the silicoaluminophosphate SAPO‐34 (CHA) and various aluminosilicate zeolites (MFI, *BEA, and FAU) with tunable acidities by a facile incipient wetness impregnation method. Evidenced by high‐resolution scanning transmission electron microscopy, the sub‐nanometric Ru clusters are uniformly distributed throughout the zeolite crystals. The X‐ray absorption spectroscopy measurements reveal the existence of Ru‐H species between Ru clusters and adjacent Brønsted acid sites of zeolites, which could synergistically activate AB and water molecules, significantly enhancing the hydrogen evolution rate of AB hydrolysis. Notably, the Ru/SAPO‐34‐0.8Si (Si/Al = 0.8) and Ru/FAU (Si/Al = 30) catalysts with strong acidities afford high turnover frequency values up to 490 and 627 min−1, respectively. These values are more than a 13‐fold enhancement than that of the commercial Ru/C catalyst, and among the top level over other heterogeneous catalysts tested under similar conditions.Keywords
Funding Information
- National Natural Science Foundation of China (21835002, 21621001)
- Argonne National Laboratory
- U.S. Department of Energy (DE‐AC02‐06CH11357)
This publication has 49 references indexed in Scilit:
- Graphene-Supported Ag-Based Core–Shell Nanoparticles for Hydrogen Generation in Hydrolysis of Ammonia Borane and Methylamine BoraneACS Applied Materials & Interfaces, 2013
- Ruthenium(0) Nanoparticles Supported on Multiwalled Carbon Nanotube As Highly Active Catalyst for Hydrogen Generation from Ammonia–BoraneACS Applied Materials & Interfaces, 2012
- Catalytic hydrolysis of ammonia borane for chemical hydrogen storageCatalysis Today, 2011
- Proton Transfer Mediated by Water: Experimental Evidence by Neutron DiffractionThe Journal of Physical Chemistry C, 2010
- Sodium borohydride versus ammonia borane, in hydrogen storage and direct fuel cell applicationsEnergy & Environmental Science, 2009
- Hydrogen and fuel cells: Towards a sustainable energy futureEnergy Policy, 2008
- Ammonia borane as an efficient and lightweight hydrogen storage mediumEnergy & Environmental Science, 2008
- Acid Initiation of Ammonia–Borane Dehydrogenation for Hydrogen StorageAngewandte Chemie, 2007
- Recent Advances in Hydrogen Storage in Metal‐Containing Inorganic Nanostructures and Related MaterialsAdvanced Materials, 2004
- Hydrogen Storage in Microporous Metal-Organic FrameworksScience, 2003