Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 40, Pages 14277-14284Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b08523
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Funding
- Ministry of Science and Technology of China [2016YFA0200700, 2016YFE0105700]
- National Natural Science Foundation of China [21373264, 21573275]
- Natural Science Foundation of Jiangsu Province [BK20150362]
- Suzhou Institute of Nanotech and Nanobionics [Y3AAA11004]
- Thousand Youth Talents Plan [Y3BQA11001]
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Gas-generating catalysis is important to many energy-related research fields, such as photocatalytic water splitting, water electrolysis, etc. The technique of single-nanoparticle catalysis is an effective way to search for highly active nanocatalysts and elucidate the reaction mechanism. However, gas-generating catalysis remains difficult to investigate at the single-nanoparticle level because product gases, such as H-2 and O-2, are difficult to detect on an individual nanoparticle. Here, we successfully find that nanobubbles can be used to study the gas-generating catalysis, i.e., H-2 generation from formic acid dehydrogenation on a single Pd-Ag nanoplate, with a high time resolution (50 ms) via dark-field microscopy. The research reveals that the nanobubble evolution process includes nucleation time and lifetime. The nucleation rate of nanobubbles is proportional to the catalytic activity of a single nanocatalyst. The relationship between the catalytic activity and the nucleation rate is quantitatively described by a mathematical model, which shows that an onset reaction rate (r(onset)) exists for the generation of nanobubbles on a single Pd-Ag nanoplate. The research also reveals that a Pd-Ag nanoplate with larger size usually has a higher activity. However, some large-sized ones still have low activities, indicating the size of the Pd-Ag nanoplate is not the only key factor for the activity. Notablely, further research shows that Pd content is the key factor for the activity of single Pd-Ag nanoplates with similar size. The methodology and knowledge acquired from this research are also applicable to other important gas-generating catalysis reactions at the single-nanoparticle level.
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