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Title: Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area

Abstract

Using renewable electricity to convert CO/CO2 into liquid products is touted as a sustainable process to produce fuels and chemicals, yet requires further advances in electrocatalyst understanding, development and device integration. The roughness factor of an electrode has generally been used to increase total rates of production, although rarely as a means to improve selectivity. In this study, we demonstrate that increasing the roughness factor of Cu electrodes is an effective design principle to direct the selectivity of CO reduction towards multicarbon oxygenates at low overpotentials and concurrently suppressing hydrocarbon and hydrogen production. The nanostructured Cu electrodes are capable of achieving almost full selectivity towards multicarbon oxygenates at an electrode potential of only –0.23 V versus the reversible hydrogen electrode. Lastly, the successful implementation of this catalytic system has enabled an excellent CO reduction performance and elucidated viable pathways to improve the energy efficiency towards liquid fuels in high-power conversion electrolysers.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [3]; ORCiD logo [4]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); McMaster Univ., Hamilton, ON (Canada)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Stanford Univ., 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)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1560654
Grant/Contract Number:  
AC02-76SF00515; SC0004993
Resource Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 2; Journal Issue: 8; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 30 DIRECT ENERGY CONVERSION

Citation Formats

Wang, Lei, Nitopi, Stephanie, Wong, Andrew B., Snider, Jonathan L., Nielander, Adam C., Morales-Guio, Carlos G., Orazov, Marat, Higgins, Drew C., Hahn, Christopher, and Jaramillo, Thomas F. Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area. United States: N. p., 2019. Web. doi:10.1038/s41929-019-0301-z.
Wang, Lei, Nitopi, Stephanie, Wong, Andrew B., Snider, Jonathan L., Nielander, Adam C., Morales-Guio, Carlos G., Orazov, Marat, Higgins, Drew C., Hahn, Christopher, & Jaramillo, Thomas F. Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area. United States. https://doi.org/10.1038/s41929-019-0301-z
Wang, Lei, Nitopi, Stephanie, Wong, Andrew B., Snider, Jonathan L., Nielander, Adam C., Morales-Guio, Carlos G., Orazov, Marat, Higgins, Drew C., Hahn, Christopher, and Jaramillo, Thomas F. Mon . "Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area". United States. https://doi.org/10.1038/s41929-019-0301-z. https://www.osti.gov/servlets/purl/1560654.
@article{osti_1560654,
title = {Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area},
author = {Wang, Lei and Nitopi, Stephanie and Wong, Andrew B. and Snider, Jonathan L. and Nielander, Adam C. and Morales-Guio, Carlos G. and Orazov, Marat and Higgins, Drew C. and Hahn, Christopher and Jaramillo, Thomas F.},
abstractNote = {Using renewable electricity to convert CO/CO2 into liquid products is touted as a sustainable process to produce fuels and chemicals, yet requires further advances in electrocatalyst understanding, development and device integration. The roughness factor of an electrode has generally been used to increase total rates of production, although rarely as a means to improve selectivity. In this study, we demonstrate that increasing the roughness factor of Cu electrodes is an effective design principle to direct the selectivity of CO reduction towards multicarbon oxygenates at low overpotentials and concurrently suppressing hydrocarbon and hydrogen production. The nanostructured Cu electrodes are capable of achieving almost full selectivity towards multicarbon oxygenates at an electrode potential of only –0.23 V versus the reversible hydrogen electrode. Lastly, the successful implementation of this catalytic system has enabled an excellent CO reduction performance and elucidated viable pathways to improve the energy efficiency towards liquid fuels in high-power conversion electrolysers.},
doi = {10.1038/s41929-019-0301-z},
journal = {Nature Catalysis},
number = 8,
volume = 2,
place = {United States},
year = {Mon Jun 17 00:00:00 EDT 2019},
month = {Mon Jun 17 00:00:00 EDT 2019}
}

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