Journal
CHEMCATCHEM
Volume 6, Issue 6, Pages 1617-1625Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201400042
Keywords
cobalt; graphene; hydrolysis; nanoparticles; silver
Categories
Funding
- National Natural Science Foundation of China [21201134]
- Natural Science Foundation of Jiangsu Province [BK20130370]
- Natural Science Foundation of Hubei Province [2013CFB288]
- Large-scale Instrument and Equipment Sharing Foundation of Wuhan University
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Tetrametallic core-shell Ag@CoNiFe nanoparticles (NPs) supported on graphene have been synthesized by a facile one-step in situ procedure for the first time. We tuned the reducing ability of the reductants to control the structure and particle size of the as-synthesized NPs. The use of weaker reducing agents, such as ammonia borane (AB) and methylamine borane (MeAB), result in the core-shell structure, whereas the stronger reducing agent NaBH4 results in alloy NPs. The as-synthesized core-shell NPs reduced by MeAB possess a smaller particle size and exhibit a superior catalytic activity compared to the core-shell NPs reduced by AB and alloy NPs reduced by NaBH4 for the hydrolytic dehydrogenation of AB. Moreover, the turnover frequency of the as-synthesized tetrametallic core-shell NPs is 118.5 mol(H2) min(-1)mol(Ag)(-1), which is higher than that of Ag-based trimetallic, bimetallic core-shell, and alloy counterparts and even higher than that of most reported noble-metal-based NPs. Kinetic studies indicate that the catalytic hydrolysis of AB and MeAB by the Ag@CoNiFe/graphene NPs is a first-order reaction. Furthermore, the as-prepared NPs exert good catalytic activities and recycle stabilities towards the hydrolysis of AB. Additionally, the as-prepared NPs display magnetic recyclability, which makes the practical recycling of the NPs more convenient.
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