期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 112, 期 29, 页码 8959-8964出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1502005112
关键词
single-molecule nanocatalysis; optical superresolution imaging; photocatalysis; surface restructuring
资金
- National Basic Research Program of China (973 Program) [2012CB932800, 2014CB932700]
- National Natural Science Foundation of China [21273220, 21303180, 201422307]
- The Recruitment Program of Global Youth Experts of China
- Light-Material Interactions in Energy Conversion, an Energy Frontier Research Center - US Department of Energy (DOE) Office of Science [DE-SC0001293]
- DOE Office of Science Graduate Fellowship Program (DOE SCGF) [DEAC05-06OR23100]
For the practical application of nanocatalysts, it is desirable to understand the spatiotemporal fluctuations of nanocatalytic activity at the single-nanoparticle level. Here we use time-lapsed superresolution mapping of single-molecule catalysis events on individual nanoparticles to observe time-varying changes in the spatial distribution of catalysis events on Sb-doped TiO2 nanorods and Au triangle nanoplates. Compared with the active sites on well-defined surface facets, the defects of the nanoparticle catalysts possess higher intrinsic reactivity but lower stability. Corners and ends are more reactive but also less stable than flat surfaces. Averaged over time, the most stable sites dominate the total apparent activity of single nanocatalysts. However, the active sites with higher intrinsic activity but lower stability show activity at earlier time points before deactivating. Unexpectedly, some active sites are found to recover their activity (self-healing) after deactivation, which is probably due to desorption of the adsorbate. Our superresolution measurement of different types of active catalytic sites, over both space and time, leads to a more comprehensive understanding of reactivity patterns and may enable the design of new and more productive heterogeneous catalysts.
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