Title

Particle Size Effects in the Catalytic Electroreduction of CO2 on Cu Nanoparticles

Authors

Authors

R. Reske; H. Mistry; F. Behafarid; B. R. Cuenya;P. Strasser

Comments

Authors: contact us about adding a copy of your work at STARS@ucf.edu

Abbreviated Journal Title

J. Am. Chem. Soc.

Keywords

OXYGEN REDUCTION REACTION; SUPPORTED RU CATALYSTS; LOW-TEMPERATURE; OXIDATION; BLOCK-COPOLYMER MICELLES; ELECTROCHEMICAL REDUCTION; PLATINUM; NANOPARTICLES; CARBON-DIOXIDE; SELECTIVE METHANATION; STRUCTURE; SENSITIVITY; ELECTRONIC-PROPERTIES; Chemistry, Multidisciplinary

Abstract

A study of particle size effects during the catalytic CO2 electroreduction on size-controlled Cu nanoparticles (NPs) is presented. Cu NP catalysts in the 2-15 nm mean size range were prepared, and their catalytic activity and selectivity during CO2 electroreduction were analyzed and compared to a bulk Cu electrode. A dramatic increase in the catalytic activity and selectivity for H-2 and CO was observed with decreasing Cu particle size, in particular, for NPs below 5 nm. Hydrocarbon (methane and ethylene) selectivity was increasingly suppressed for nanoscale Cu surfaces. The size dependence of the surface atomic coordination of model spherical Cu particles was used to rationalize the experimental results. Changes in the population of low-coordinated surface sites and their stronger chemisorption were linked to surging H-2 and CO selectivities, higher catalytic activity, and smaller hydrocarbon selectivity. The presented activity-selectivity-size relations provide novel insights in the CO2 electroreduction reaction on nanoscale surfaces. Our smallest nanoparticles (similar to 2 nm) enter the ab initio computationally accessible size regime, and therefore, the results obtained lend themselves well to density functional theory (DFT) evaluation and reaction mechanism verification.

Journal Title

Journal of the American Chemical Society

Volume

136

Issue/Number

19

Publication Date

1-1-2014

Document Type

Article

Language

English

First Page

6978

Last Page

6986

WOS Identifier

WOS:000336078400042

ISSN

0002-7863

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