Vapor–Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel–Coordinated Nitrogen–Doped Carbon
Abstract
We report ethylene is particularly attractive due to its major importance as a feedstock for various applications including the polymer industry. As such, catalyst and electrolyzer developments are crucial to achieve industrially relevant ethylene production and efficiency levels. In this work, a tandem electrocatalyst composed of copper nanocubes and nickel-coordinated nitrogen-doped carbon (NiNC) is presented, which is integrated into gas diffusion electrodes (GDEs) for direct conversion of vapor-fed CO2 into ethylene. Evaluation of tandem GDEs in the vapor-fed flow electrolyzer shows significantly increased ethylene selectivity in terms of faradaic efficiency and C2H4/CO ratio compared to a non-tandem copper GDE. The enhancements are attributed to the increased local CO availability near the copper surface via effective CO2 to CO conversion on neighboring NiNC. The experimental results are validated by 3D resolved continuum simulations, which show increased flux of higher-order prod-ucts with the added CO flux from NiNC. The practical viability of Cu/NiNC catalyst is further evaluated in a membrane electrode assembly electrolyzer, achieving 40% FE toward ethylene at 150 mA cm-2 and 3.2 V. These find-ings highlight the high selectivity and formation rate of ethylene achieved by successful device integration of the Cu/NiNC catalyst, demonstrating the potential for implementation in large-scalemore »
- Authors:
-
- Stanford University, CA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Stanford University, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Ministry of Science and technology (MOST); National Science Foundation (NSF)
- OSTI Identifier:
- 1874000
- Grant/Contract Number:
- AC02-76SF00515; ECCS-2026822
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 32; Journal Issue: 28; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; CO2 reduction; electrocatalysis; ethylene; membrane electrode assemblies; MEA; selectivity; tandem catalysis
Citation Formats
Lin, Yi‐Rung, Lee, Dong Un, Tan, Shunquan, Koshy, David M., Lin, Tiras Y., Wang, Lei, Corral, Daniel, Avilés Acosta, Jaime E., Zamora Zeledon, Jose A., Beck, Victor A., Baker, Sarah E., Duoss, Eric B., Hahn, Christopher, and Jaramillo, Thomas F. Vapor–Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel–Coordinated Nitrogen–Doped Carbon. United States: N. p., 2022.
Web. doi:10.1002/adfm.202113252.
Lin, Yi‐Rung, Lee, Dong Un, Tan, Shunquan, Koshy, David M., Lin, Tiras Y., Wang, Lei, Corral, Daniel, Avilés Acosta, Jaime E., Zamora Zeledon, Jose A., Beck, Victor A., Baker, Sarah E., Duoss, Eric B., Hahn, Christopher, & Jaramillo, Thomas F. Vapor–Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel–Coordinated Nitrogen–Doped Carbon. United States. https://doi.org/10.1002/adfm.202113252
Lin, Yi‐Rung, Lee, Dong Un, Tan, Shunquan, Koshy, David M., Lin, Tiras Y., Wang, Lei, Corral, Daniel, Avilés Acosta, Jaime E., Zamora Zeledon, Jose A., Beck, Victor A., Baker, Sarah E., Duoss, Eric B., Hahn, Christopher, and Jaramillo, Thomas F. Wed .
"Vapor–Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel–Coordinated Nitrogen–Doped Carbon". United States. https://doi.org/10.1002/adfm.202113252. https://www.osti.gov/servlets/purl/1874000.
@article{osti_1874000,
title = {Vapor–Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel–Coordinated Nitrogen–Doped Carbon},
author = {Lin, Yi‐Rung and Lee, Dong Un and Tan, Shunquan and Koshy, David M. and Lin, Tiras Y. and Wang, Lei and Corral, Daniel and Avilés Acosta, Jaime E. and Zamora Zeledon, Jose A. and Beck, Victor A. and Baker, Sarah E. and Duoss, Eric B. and Hahn, Christopher and Jaramillo, Thomas F.},
abstractNote = {We report ethylene is particularly attractive due to its major importance as a feedstock for various applications including the polymer industry. As such, catalyst and electrolyzer developments are crucial to achieve industrially relevant ethylene production and efficiency levels. In this work, a tandem electrocatalyst composed of copper nanocubes and nickel-coordinated nitrogen-doped carbon (NiNC) is presented, which is integrated into gas diffusion electrodes (GDEs) for direct conversion of vapor-fed CO2 into ethylene. Evaluation of tandem GDEs in the vapor-fed flow electrolyzer shows significantly increased ethylene selectivity in terms of faradaic efficiency and C2H4/CO ratio compared to a non-tandem copper GDE. The enhancements are attributed to the increased local CO availability near the copper surface via effective CO2 to CO conversion on neighboring NiNC. The experimental results are validated by 3D resolved continuum simulations, which show increased flux of higher-order prod-ucts with the added CO flux from NiNC. The practical viability of Cu/NiNC catalyst is further evaluated in a membrane electrode assembly electrolyzer, achieving 40% FE toward ethylene at 150 mA cm-2 and 3.2 V. These find-ings highlight the high selectivity and formation rate of ethylene achieved by successful device integration of the Cu/NiNC catalyst, demonstrating the potential for implementation in large-scale sustainable CO2 electrolyzers.},
doi = {10.1002/adfm.202113252},
journal = {Advanced Functional Materials},
number = 28,
volume = 32,
place = {United States},
year = {Wed May 11 00:00:00 EDT 2022},
month = {Wed May 11 00:00:00 EDT 2022}
}
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