期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 24, 期 47, 页码 12330-12339出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201705749
关键词
gold; hydrogenation; nanocatalysis; nanoparticles; surface plasmon resonance
资金
- FAPESP [2015/21366-9, 2015/26308-7, 2016/16738-7, 2015/11452-5]
- CNPq
- CAPES
The localized surface plasmon resonance (LSPR) excitation in plasmonic nanoparticles can enhance or mediate chemical transformations. Increased reaction rates for several reactions have been reported due to this phenomenon; however, the fundamental understanding of mechanisms and factors that affect activities remains limited. Here, by investigating hydrogenation reactions as a model transformation and employing different reducing agents, H-2 and NaBH4, which led to different hydrogenation reaction pathways, we observed that plasmonic excitation of Au nanoparticle catalysts can lead to negative effects over the activities. The underlying physical reason was explored using density functional theory calculations. We observed that positive versus negative effects on the plasmonic catalytic activity is reaction-pathway dependent. These results shed important insights on our current understanding of plasmonic catalysis, demonstrating reaction pathways must be taken into account for the design of plasmonic nanocatalysts.
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