@article{e565f6fe245243acbf83e12212c809de,
title = "Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging",
abstract = "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.",
author = "Guanqun Chen and Ningmu Zou and Bo Chen and Sambur, {Justin B.} and Eric Choudhary and Peng Chen",
note = "Funding Information: This research is supported mainly by the Army Research Office (W911NF-14-1-0377) and in part by the Department of Energy (DE-SC0004911), Army Research Office (W911NF-14-1-0620), and National Science Foundation (CBET1263736). This work made use of the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC program DMR1120296) and of the Cornell NanoScale Facility, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), supported by the National Science Foundation (ECCS1542081). B.C. and the computational facilities used in this work at Cornell are supported by the Energy Frontier Research in Extreme Environments (EFree) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DE-SC0001057). Funding Information: We thank Roald Hoffmann for access to computational facilities and comments, Tai-Yen Chen for providing Matlab codes, and Xiaochun Zhou and Hao Shen for assistance in microscopy setups. This research is supported mainly by the Army Research Office (W911NF-14-1-0377) and in part by the Department of Energy (DE-SC0004911), Army Research Office (W911NF-14-1-0620), and National Science Foundation (CBET1263736). This work made use of the Cornell Center for Materials Research Shared Facilities, which are supported through the NSF MRSEC program (DMR1120296), and of the Cornell NanoScale Facility, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), supported by the National Science Foundation (ECCS1542081). B.C. and the computational facilities used in this work at Cornell are supported by the Energy Frontier Research in Extreme Environments (EFree) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DE-SC0001057). Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",
year = "2017",
month = nov,
day = "22",
doi = "10.1021/acscentsci.7b00377",
language = "English (US)",
volume = "3",
pages = "1189--1197",
journal = "ACS Central Science",
issn = "2374-7943",
publisher = "American Chemical Society",
number = "11",
}