Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity | |
Zhang,Yuwei; Lucas,J.Matthew; Song,Ping; Beberwyck,Brandon; Fu,Qiang; Xu,Weilin; Alivisatos,A.Paul | |
刊名 | proceedings of the national academy of sciences of the united states of america |
2015 | |
卷号 | 112期号:29页码:8959-8964 |
关键词 | MOLECULAR-DYNAMICS SIMULATION CO OXIDATION NANOCATALYSTS NANOCRYSTALS MICROSCOPY SITES TIME HETEROGENEITIES PHOTOCATALYSIS SPECTROSCOPY |
通讯作者 | alivisatos, ap |
英文摘要 | 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. |
收录类别 | SCI |
语种 | 英语 |
WOS记录号 | WOS:000358225100058 |
内容类型 | 期刊论文 |
源URL | [http://ir.ciac.jl.cn/handle/322003/64570] |
专题 | 长春应用化学研究所_长春应用化学研究所知识产出_期刊论文 |
推荐引用方式 GB/T 7714 | Zhang,Yuwei,Lucas,J.Matthew,Song,Ping,et al. Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity[J]. proceedings of the national academy of sciences of the united states of america,2015,112(29):8959-8964. |
APA | Zhang,Yuwei.,Lucas,J.Matthew.,Song,Ping.,Beberwyck,Brandon.,Fu,Qiang.,...&Alivisatos,A.Paul.(2015).Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity.proceedings of the national academy of sciences of the united states of america,112(29),8959-8964. |
MLA | Zhang,Yuwei,et al."Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity".proceedings of the national academy of sciences of the united states of america 112.29(2015):8959-8964. |
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