The importance of nanoscale confinement to electrocatalytic performance.

Chemical Science
Johanna WordsworthJ Justin Gooding

Abstract

Electrocatalytic nanoparticles that mimic the three-dimensional geometric architecture of enzymes where the reaction occurs down a substrate channel isolated from bulk solution, referred to herein as nanozymes, were used to explore the impact of nano-confinement on electrocatalytic reactions. Surfactant covered Pt-Ni nanozyme nanoparticles, with Ni etched from the nanoparticles, possess a nanoscale channel in which the active sites for electrocatalysis of oxygen reduction are located. Different particle compositions and etching parameters allowed synthesis of nanoparticles with different average substrate channel diameters that have varying amounts of nano-confinement. The results showed that in the kinetically limited regime at low overpotentials, the smaller the substrate channels the higher the specific activity of the electrocatalyst. This is attributed to higher concentrations of protons, relative to bulk solution, required to balance the potential inside the nano-confined channel. However, at higher overpotentials where limitation by mass transport of oxygen becomes important, the nanozymes with larger substrate channels showed higher electrocatalytic activity. A reaction-diffusion model revealed that the higher electroca...Continue Reading

References

Jan 16, 2007·Science·Vojislav R StamenkovicNenad M Marković
Oct 19, 2010·Nature Materials·J SnyderJ Erlebacher
Sep 25, 2018·Journal of the American Chemical Society·Tania M BenedettiJ Justin Gooding

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Citations

Jun 25, 2021·Chemical Science·Valentina DichiaranteFrancesca Baldelli Bombelli
Jan 13, 2021·Sensors·Elicia L S WongEdith Chow
Jul 7, 2020·Journal of the American Chemical Society·Jaeyune Ryu, Yogesh Surendranath

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Methods Mentioned

BETA
X-ray

Software Mentioned

Comsol
Comsol Multiphysics
Nova

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