Underlying Mechanisms of Hot Carrier-Driven Reactivity on Bimetallic Nanostructures

Li, Zhandong; Rigor, Joel; Large, Nicolas; El-Khoury, Patrick Z.; Kurouski, Dmitry

doi:10.1021/acs.jpcc.1c00155

Title: Underlying Mechanisms of Hot Carrier-Driven Reactivity on Bimetallic Nanostructures

Journal Article · Thu Feb 04 00:00:00 EST 2021 · Journal of Physical Chemistry C

DOI:https://doi.org/10.1021/acs.jpcc.1c00155· OSTI ID:1768868

Li, Zhandong ^[1]; Rigor, Joel ^[2]; Large, Nicolas ^[2];

^[3]; Kurouski, Dmitry ^[1]

Texas A & M University
University of Texas
BATTELLE (PACIFIC NW LAB)

Bimetallic nanostructures exhibit unique catalytic activity and selectivity that is not evident for their monometallic analogs. Such nanostructures contain plasmonic metals, such as gold or silver, that afford highly efficient harvesting of electromagnetic radiation and its conversion into hot carriers. These highly energetic species are transferred to the catalytic metal sub-component of the bimetallic nanostructure, where a large spectrum of chemical reactions may be catalyzed. The strength of the electric field and the interplay between catalytic and plasmonic metals at the nanoscale are thus critically important for the catalytic activity of bimetallic nanostructures. In this study, we investigate the relationship between the catalytic activity and local electric fields sustained on the surface of gold-palladium (Au@PdNPs) and gold-platinum (Au@PtNPs) nanoplates using tip-enhanced Raman spectroscopy (TERS). We image the spatially varying magnitudes of rectified (DC) local electric fields on the surface of these nanostructures and compare them to fields sustained on the surface of monometallic nanoplates. We find substantially larger electric field magnitudes on Au@PdNPs and Au@PtNPs as compared to their monometallic analogs. These findings suggest that catalytic efficiency of bimetallic nanostructures may be mediated and potentially tuned through precise control of electric fields sustained on their surfaces.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1768868

Report Number(s):: PNNL-SA-159335

Journal Information:: Journal of Physical Chemistry C, Vol. 125, Issue 4

Country of Publication:: United States

Language:: English

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