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

Chen, Guanqun; Zou, Ningmu; Chen, Bo; Sambur, Justin B.; Choudhary, Eric; Chen, Peng

doi:10.1021/acscentsci.7b00377

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

Journal Article · Wed Nov 01 00:00:00 EDT 2017 · ACS Central Science

DOI:https://doi.org/10.1021/acscentsci.7b00377· OSTI ID:1406929

Chen, Guanqun ^[1]; Zou, Ningmu ^[1];

^[1]; Sambur, Justin B. ^[1]; Choudhary, Eric ^[1];

^[1]

Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14853, United States

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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Research Organization:: Cornell Univ., Ithaca, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (EFree)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001057; SC0004911

OSTI ID:: 1406929

Alternate ID(s):: OSTI ID: 1417631; OSTI ID: 1507709

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Vol. 3 Journal Issue: 11; ISSN 2374-7943

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 50 works

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