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Title: Copper nanoparticle ensembles for selective electroreduction of CO 2 to C 2-C 3 products

Abstract

Direct conversion of carbon dioxide to multicarbon products remains as a grand challenge in electrochemical CO 2 reduction. Various forms of oxidized copper have been demonstrated as electrocatalysts that still require large overpotentials. Here in this paper, we show that an ensemble of Cu nanoparticles (NPs) enables selective formation of C 2–C 3 products at low overpotentials. Densely packed Cu NP ensembles underwent structural transformation during electrolysis into electrocatalytically active cube-like particles intermixed with smaller nanoparticles. Ethylene, ethanol, and n-propanol are the major C 2–C 3 products with onset potential at -0.53 V (vs. reversible hydrogen electrode, RHE) and C 2–C 3 faradaic efficiency (FE) reaching 50% at only -0.75 V. Thus, the catalyst exhibits selective generation of C 2–C 3 hydrocarbons and oxygenates at considerably lowered overpotentials in neutral pH aqueous media. In addition, this approach suggests new opportunities in realizing multicarbon product formation from CO 2, where the majority of efforts has been to use oxidized copper-based materials. Robust catalytic performance is demonstrated by 10 h of stable operation with C 2–C 3 current density 10 mA/cm 2 (at -0.75 V), rendering it attractive for solar-to-fuel applications. Lastly, Tafel analysis suggests reductive CO coupling as a rate determiningmore » step for C 2 products, while n-propanol (C 3) production seems to have a discrete pathway.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4]
  1. Univ. of California, Berkeley, CA (United States). Department of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Kavli Energy NanoScience Institute, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States). Department of Chemistry
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Kavli Energy NanoScience Institute, Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States). Department of Chemistry
  4. Univ. of California, Berkeley, CA (United States). Department of Materials Science and Engineering and Department of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Kavli Energy NanoScience Institute, 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). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1392689
Alternate Identifier(s):
OSTI ID: 1426737
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 40; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 30 DIRECT ENERGY CONVERSION; heterogeneous catalysis; electrocatalysis; CO2 reduction; copper nanoparticles; in situ structural transformation

Citation Formats

Kim, Dohyung, Kley, Christopher S., Li, Yifan, and Yang, Peidong. Copper nanoparticle ensembles for selective electroreduction of CO2 to C2-C3 products. United States: N. p., 2017. Web. doi:10.1073/pnas.1711493114.
Kim, Dohyung, Kley, Christopher S., Li, Yifan, & Yang, Peidong. Copper nanoparticle ensembles for selective electroreduction of CO2 to C2-C3 products. United States. doi:10.1073/pnas.1711493114.
Kim, Dohyung, Kley, Christopher S., Li, Yifan, and Yang, Peidong. Mon . "Copper nanoparticle ensembles for selective electroreduction of CO2 to C2-C3 products". United States. doi:10.1073/pnas.1711493114.
@article{osti_1392689,
title = {Copper nanoparticle ensembles for selective electroreduction of CO2 to C2-C3 products},
author = {Kim, Dohyung and Kley, Christopher S. and Li, Yifan and Yang, Peidong},
abstractNote = {Direct conversion of carbon dioxide to multicarbon products remains as a grand challenge in electrochemical CO2 reduction. Various forms of oxidized copper have been demonstrated as electrocatalysts that still require large overpotentials. Here in this paper, we show that an ensemble of Cu nanoparticles (NPs) enables selective formation of C2–C3 products at low overpotentials. Densely packed Cu NP ensembles underwent structural transformation during electrolysis into electrocatalytically active cube-like particles intermixed with smaller nanoparticles. Ethylene, ethanol, and n-propanol are the major C2–C3 products with onset potential at -0.53 V (vs. reversible hydrogen electrode, RHE) and C2–C3 faradaic efficiency (FE) reaching 50% at only -0.75 V. Thus, the catalyst exhibits selective generation of C2–C3 hydrocarbons and oxygenates at considerably lowered overpotentials in neutral pH aqueous media. In addition, this approach suggests new opportunities in realizing multicarbon product formation from CO2, where the majority of efforts has been to use oxidized copper-based materials. Robust catalytic performance is demonstrated by 10 h of stable operation with C2–C3 current density 10 mA/cm2 (at -0.75 V), rendering it attractive for solar-to-fuel applications. Lastly, Tafel analysis suggests reductive CO coupling as a rate determining step for C2 products, while n-propanol (C3) production seems to have a discrete pathway.},
doi = {10.1073/pnas.1711493114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 40,
volume = 114,
place = {United States},
year = {Mon Sep 18 00:00:00 EDT 2017},
month = {Mon Sep 18 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1073/pnas.1711493114

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Cited by: 17 works
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Works referenced in this record:

Electrochemical reduction of carbon dioxide at various series of copper single crystal electrodes
journal, May 2003