期刊
ACS CENTRAL SCIENCE
卷 3, 期 11, 页码 1189-1197出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.7b00377
关键词
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资金
- Army Research Office [W911NF-14-1-0377, W911NF-14-1-0620]
- Department of Energy [DE-SC0004911]
- National Science Foundation [CBET1263736, ECCS1542081]
- NSF MRSEC [DMR1120296]
- Energy Frontier Research in Extreme Environments (EFree) Center, an Energy Frontier Research Center - U.S. Department of Energy [DE-SC0001057]
- U.S. Department of Energy (DOE) [DE-SC0004911] Funding Source: U.S. Department of Energy (DOE)
Compared with their monometallic counterparts, bimetallic nanoparticles often show enhanced catalytic activity associated with the bimetallic interface. Direct quantitation of catalytic activity at the bimetallic interface is important for understanding the enhancement mechanism, but challenging experimentally. Here using single-molecule super-resolution catalysis imaging in correlation with electron microscopy, we report the first quantitative visualization of enhanced bimetallic activity within single bimetallic nanoparticles. We focus on heteronuclear bimetallic PdAu nanoparticles that present a well-defined Pd-Au bimetallic interface in catalyzing a photodriven fluorogenic disproportionation reaction. Our approach also enables a direct comparison between the bimetallic and monometallic regions within the same nanoparticle. Theoretical calculations further provide insights into the electronic nature of N-O bond activation of the reactant (resazurin) adsorbed on bimetallic sites. Subparticle activity correlation between bimetallic enhancement and monometallic activity suggests that the favorable locations to construct bimetallic sites are those monometallic sites with higher activity, leading to a strategy for making effective bimetallic nanocatalysts. The results highlight the power of super-resolution catalysis imaging in gaining insights that could help improve nanocatalysts.
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