Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 39, Pages 11950-11954Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201604021
Keywords
graphene oxide; heterogeneous catalysis; hydrogen storage; hydrolysis mechanism; nanoparticles
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Funding
- National Basic Research Development Program of China [2012CB825800]
- National Natural Science Foundation of China [11275137, 11179032, 91333112, U1432249]
- Soochow University-Western University Centre for Synchrotron Radiation Research
- Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices
- Collaborative Innovation Center of Suzhou Nano Science Technology
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Fund for Innovative Research Teams of Jiangsu Higher Education Institutions
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Ammonia-borane (AB) is an excellent material for chemical storage of hydrogen. However, the practical utilization of AB for production of hydrogen is hindered by the need of expensive noble metal-based catalysts. Here, we report CuxCo1-xO nanoparticles (NPs) facilely deposited on graphene oxide (GO) as a low-cost and high-performance catalyst for the hydrolysis of AB. This hybrid catalyst exhibits an initial total turnover frequency (TOF) value of 70.0 (H-2) mol/(Cat-metal) mol.min, which is the highest TOF ever reported for noble metal-free catalysts, and a good stability keeping 94 % activity after 5 cycles. Synchrotron radiation-based X-ray absorption spectroscopy (XAS) investigations suggested that the high catalytic performance could be attributed to the interfacial interaction between CuxCo1-xO NPs and GO. Moreover, the catalytic hydrolysis mechanism was studied by in situ XAS experiments for the first time, which reveal a significant water adsorption on the catalyst and clearly confirm the interaction between AB and the catalyst during hydrolysis.
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