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      Bimetallic Effect of Single Nanocatalysts Visualized by Super-Resolution Catalysis Imaging

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          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.

          Abstract

          Super-resolution catalysis imaging in correlation with electron microscopy directly visualizes and quantifies catalytic enhancements at metal−metal interfaces within single bimetallic nanoparticles.

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          Most cited references39

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          Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis set

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            Density functional theory in surface chemistry and catalysis.

            Recent advances in the understanding of reactivity trends for chemistry at transition-metal surfaces have enabled in silico design of heterogeneous catalysts in a few cases. The current status of the field is discussed with an emphasis on the role of coupling theory and experiment and future challenges.
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              Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles

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                Author and article information

                Journal
                ACS Cent Sci
                ACS Cent Sci
                oc
                acscii
                ACS Central Science
                American Chemical Society
                2374-7943
                2374-7951
                01 November 2017
                22 November 2017
                : 3
                : 11
                : 1189-1197
                Affiliations
                [1]Department of Chemistry and Chemical Biology, Cornell University , Ithaca, New York 14853, United States
                Author notes
                Article
                10.1021/acscentsci.7b00377
                5704284
                29202021
                9a6afd3e-0640-4980-a76e-269d71836fab
                Copyright © 2017 American Chemical Society

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

                History
                : 15 August 2017
                Categories
                Research Article
                Custom metadata
                oc7b00377
                oc-2017-003775

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