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 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 discretemore »
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1392689
- Alternate Identifier(s):
- OSTI ID: 1426737
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America 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 CO 2 to C 2 –C 3 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 CO 2 to C 2 –C 3 products. United States. https://doi.org/10.1073/pnas.1711493114
Kim, Dohyung, Kley, Christopher S., Li, Yifan, and Yang, Peidong. Mon .
"Copper nanoparticle ensembles for selective electroreduction of CO 2 to C 2 –C 3 products". United States. https://doi.org/10.1073/pnas.1711493114.
@article{osti_1392689,
title = {Copper nanoparticle ensembles for selective electroreduction of CO 2 to C 2 –C 3 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}
}
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