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Title: Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst

Abstract

Here, the discovery of materials for the electrochemical transformation of carbon dioxide into liquid fuels has the potential to impact large-scale storage of renewable energies and reduce carbon emissions. Here, we report the discovery of an electrocatalyst composed of gold nanoparticles on a polycrystalline copper foil (Au/Cu) that is highly active for CO2 reduction to alcohols. At low overpotentials, the Au/Cu electrocatalyst is over 100 times more selective for the formation of products containing C–C bonds versus methane or methanol, largely favouring the generation of alcohols over hydrocarbons. A combination of electrochemical testing and transport modelling supports the hypothesis that CO2 reduction on gold generates a high CO concentration on nearby copper, where CO is further reduced to alcohols such as ethanol and n-propanol under locally alkaline conditions. The bimetallic Au/Cu electrocatalyst exhibits synergistic activity and selectivity superior to gold, copper or AuCu alloys, and opens new possibilities for the development of CO2 reduction electrodes exploiting tandem catalysis mechanisms.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [2]
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  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490634
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 10; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Morales-Guio, Carlos G., Cave, Etosha R., Nitopi, Stephanie A., Feaster, Jeremy T., Wang, Lei, Kuhl, Kendra P., Jackson, Ariel, Johnson, Natalie C., Abram, David N., Hatsukade, Toru, Hahn, Christopher, and Jaramillo, Thomas F. Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst. United States: N. p., 2018. Web. doi:10.1038/s41929-018-0139-9.
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Morales-Guio, Carlos G., Cave, Etosha R., Nitopi, Stephanie A., Feaster, Jeremy T., Wang, Lei, Kuhl, Kendra P., Jackson, Ariel, Johnson, Natalie C., Abram, David N., Hatsukade, Toru, Hahn, Christopher, & Jaramillo, Thomas F. Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst. United States. https://doi.org/10.1038/s41929-018-0139-9
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Morales-Guio, Carlos G., Cave, Etosha R., Nitopi, Stephanie A., Feaster, Jeremy T., Wang, Lei, Kuhl, Kendra P., Jackson, Ariel, Johnson, Natalie C., Abram, David N., Hatsukade, Toru, Hahn, Christopher, and Jaramillo, Thomas F. Thu . "Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst". United States. https://doi.org/10.1038/s41929-018-0139-9. https://www.osti.gov/servlets/purl/1490634.
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@article{osti_1490634,
title = {Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst},
author = {Morales-Guio, Carlos G. and Cave, Etosha R. and Nitopi, Stephanie A. and Feaster, Jeremy T. and Wang, Lei and Kuhl, Kendra P. and Jackson, Ariel and Johnson, Natalie C. and Abram, David N. and Hatsukade, Toru and Hahn, Christopher and Jaramillo, Thomas F.},
abstractNote = {Here, the discovery of materials for the electrochemical transformation of carbon dioxide into liquid fuels has the potential to impact large-scale storage of renewable energies and reduce carbon emissions. Here, we report the discovery of an electrocatalyst composed of gold nanoparticles on a polycrystalline copper foil (Au/Cu) that is highly active for CO2 reduction to alcohols. At low overpotentials, the Au/Cu electrocatalyst is over 100 times more selective for the formation of products containing C–C bonds versus methane or methanol, largely favouring the generation of alcohols over hydrocarbons. A combination of electrochemical testing and transport modelling supports the hypothesis that CO2 reduction on gold generates a high CO concentration on nearby copper, where CO is further reduced to alcohols such as ethanol and n-propanol under locally alkaline conditions. The bimetallic Au/Cu electrocatalyst exhibits synergistic activity and selectivity superior to gold, copper or AuCu alloys, and opens new possibilities for the development of CO2 reduction electrodes exploiting tandem catalysis mechanisms.},
doi = {10.1038/s41929-018-0139-9},
journal = {Nature Catalysis},
number = 10,
volume = 1,
place = {United States},
year = {Thu Oct 11 00:00:00 EDT 2018},
month = {Thu Oct 11 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1038/s41929-018-0139-9
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Figures / Tables:

Fig. 1 Fig. 1: Physical characterization of Au/Cu, a, SEM secondary electron images of the as-prepared Au/Cu catalyst. The brighter spots correspond to approximately 3-5 nm gold nanoparticles on a polycrystalline copper surface. b, SEM secondary electron images of Au/Cu after CO2 reduction. Scale bars in a and b: 100 nm. Scalemore » bars in insets: 20 nm. c, High-resolution XPS spectra of the copper 2$p$ and gold 4$f$ regions for Au/Cu before (as-prepared sample) and after CO2 reduction testing. d, Grazing-incidence X-ray diffractogram of the Au/Cu catalyst after CO2 reduction testing. The inset shows peaks originating from gold nanoparticles on the copper surface.« less
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