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Title: Tailoring Copper Nanocrystals towards C 2 Products in Electrochemical CO 2 Reduction

Abstract

Favoring the CO 2 reduction reaction (CO 2RR) over the hydrogen evolution reaction and controlling the selectivity towards multicarbon products are currently major scientific challenges in sustainable energy research. It is known that the morphology of the catalyst can modulate catalytic activity and selectivity, yet this remains a relatively underexplored area in electrochemical CO 2 reduction. In this study, we exploit the material tunability afforded by colloidal chemistry to establish unambiguous structure/property relations between Cu nanocrystals and their behavior as electrocatalysts for CO 2 reduction. Our study reveals a non-monotonic size-dependence of the selectivity in cube-shaped copper nanocrystals. Among 24 nm, 44 nm and 63 nm cubes tested, the cubes with 44 nm edge length exhibited the highest selectivity towards CO 2RR (80 %) and faradaic efficiency for ethylene (41 %). Finally, statistical analysis of the surface atom density suggests the key role played by edge sites in CO 2RR.

Authors:
 [1];  [2];  [1];  [3];  [3];  [2]; ORCiD logo [1]
  1. École Polytechnique Fédérale de Lausanne, Sion (Switzerland)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1530238
Alternate Identifier(s):
OSTI ID: 1401425
Grant/Contract Number:  
AC02-05CH11231; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 19; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; colloidal chemistry; electrochemical CO2 reduction; nanocrystals; nanocubes; selectivity

Citation Formats

Loiudice, Anna, Lobaccaro, Peter, Kamali, Esmail A., Thao, Timothy, Huang, Brandon H., Ager, Joel W., and Buonsanti, Raffaella. Tailoring Copper Nanocrystals towards C2 Products in Electrochemical CO2 Reduction. United States: N. p., 2016. Web. doi:10.1002/anie.201601582.
Loiudice, Anna, Lobaccaro, Peter, Kamali, Esmail A., Thao, Timothy, Huang, Brandon H., Ager, Joel W., & Buonsanti, Raffaella. Tailoring Copper Nanocrystals towards C2 Products in Electrochemical CO2 Reduction. United States. doi:10.1002/anie.201601582.
Loiudice, Anna, Lobaccaro, Peter, Kamali, Esmail A., Thao, Timothy, Huang, Brandon H., Ager, Joel W., and Buonsanti, Raffaella. Tue . "Tailoring Copper Nanocrystals towards C2 Products in Electrochemical CO2 Reduction". United States. doi:10.1002/anie.201601582. https://www.osti.gov/servlets/purl/1530238.
@article{osti_1530238,
title = {Tailoring Copper Nanocrystals towards C2 Products in Electrochemical CO2 Reduction},
author = {Loiudice, Anna and Lobaccaro, Peter and Kamali, Esmail A. and Thao, Timothy and Huang, Brandon H. and Ager, Joel W. and Buonsanti, Raffaella},
abstractNote = {Favoring the CO2 reduction reaction (CO2RR) over the hydrogen evolution reaction and controlling the selectivity towards multicarbon products are currently major scientific challenges in sustainable energy research. It is known that the morphology of the catalyst can modulate catalytic activity and selectivity, yet this remains a relatively underexplored area in electrochemical CO2 reduction. In this study, we exploit the material tunability afforded by colloidal chemistry to establish unambiguous structure/property relations between Cu nanocrystals and their behavior as electrocatalysts for CO2 reduction. Our study reveals a non-monotonic size-dependence of the selectivity in cube-shaped copper nanocrystals. Among 24 nm, 44 nm and 63 nm cubes tested, the cubes with 44 nm edge length exhibited the highest selectivity towards CO2RR (80 %) and faradaic efficiency for ethylene (41 %). Finally, statistical analysis of the surface atom density suggests the key role played by edge sites in CO2RR.},
doi = {10.1002/anie.201601582},
journal = {Angewandte Chemie (International Edition)},
number = 19,
volume = 55,
place = {United States},
year = {2016},
month = {4}
}

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Works referenced in this record:

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