Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
Abstract
A strategy to modulate the electrocatalytic activity of copper toward CO2 reduction involving adsorption of acrylamide, acrylic acid, and allylamine polymers is presented. Modification of electrodeposited copper foam with poly(acrylamide) leads to a significant enhancement in faradaic efficiency for ethylene from 13% (unmodified foam) to 26% at -0.96 V vs RHE, whereas methane yield is unaffected. Effects from crystalline phase distribution and copper oxide phases are ruled out as the source of enhancement through XPS and in situ XRD analysis. DFT calculations reveal that poly(acrylamide) adsorbs on the copper surface via the oxygen atom on the carbonyl groups and enhances ethylene formation by (i) charge donation to the copper surface that activates CO for dimerization, (ii) chemical stabilization of the CO dimer (a key intermediate for C2 products) by hydrogen-bond interactions with the -NH2 group, and (iii) facilitating the adsorption of CO molecules near the polymer, increasing local surface coverage. Poly(acrylamide) with copper acts as a multipoint binding catalytic system where the interplay between activation and stabilization of intermediates results in enhanced selectivity toward ethylene formation. Finally, modification with poly(acrylic acid) which has a similar structure to poly(acrylamide) also shows some enhancement in activity but is unstable, whereas poly(allylamine) completelymore »
- Authors:
-
- Swansea Univ., Swansea (United Kingdom). Energy Safety Research Inst.
- Univ. of Nebraska-Lincoln, Lincoln, NE (United States). Dept. of Chemical and Biomolecular Engineering
- European Synchrotron Radiation Facility, Grenoble (France)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1543699
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 5; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; electrocatalysis; greenhouse gas; heterogeneous catalyst; modified electrodes; ethylene; DFT; blue moon
Citation Formats
Ahn, Sunyhik, Klyukin, Konstantin, Wakeham, Russell J., Rudd, Jennifer A., Lewis, Aled R., Alexander, Shirin, Carla, Francesco, Alexandrov, Vitaly, and Andreoli, Enrico. Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide. United States: N. p., 2018.
Web. doi:10.1021/acscatal.7b04347.
Ahn, Sunyhik, Klyukin, Konstantin, Wakeham, Russell J., Rudd, Jennifer A., Lewis, Aled R., Alexander, Shirin, Carla, Francesco, Alexandrov, Vitaly, & Andreoli, Enrico. Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide. United States. https://doi.org/10.1021/acscatal.7b04347
Ahn, Sunyhik, Klyukin, Konstantin, Wakeham, Russell J., Rudd, Jennifer A., Lewis, Aled R., Alexander, Shirin, Carla, Francesco, Alexandrov, Vitaly, and Andreoli, Enrico. Tue .
"Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide". United States. https://doi.org/10.1021/acscatal.7b04347. https://www.osti.gov/servlets/purl/1543699.
@article{osti_1543699,
title = {Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide},
author = {Ahn, Sunyhik and Klyukin, Konstantin and Wakeham, Russell J. and Rudd, Jennifer A. and Lewis, Aled R. and Alexander, Shirin and Carla, Francesco and Alexandrov, Vitaly and Andreoli, Enrico},
abstractNote = {A strategy to modulate the electrocatalytic activity of copper toward CO2 reduction involving adsorption of acrylamide, acrylic acid, and allylamine polymers is presented. Modification of electrodeposited copper foam with poly(acrylamide) leads to a significant enhancement in faradaic efficiency for ethylene from 13% (unmodified foam) to 26% at -0.96 V vs RHE, whereas methane yield is unaffected. Effects from crystalline phase distribution and copper oxide phases are ruled out as the source of enhancement through XPS and in situ XRD analysis. DFT calculations reveal that poly(acrylamide) adsorbs on the copper surface via the oxygen atom on the carbonyl groups and enhances ethylene formation by (i) charge donation to the copper surface that activates CO for dimerization, (ii) chemical stabilization of the CO dimer (a key intermediate for C2 products) by hydrogen-bond interactions with the -NH2 group, and (iii) facilitating the adsorption of CO molecules near the polymer, increasing local surface coverage. Poly(acrylamide) with copper acts as a multipoint binding catalytic system where the interplay between activation and stabilization of intermediates results in enhanced selectivity toward ethylene formation. Finally, modification with poly(acrylic acid) which has a similar structure to poly(acrylamide) also shows some enhancement in activity but is unstable, whereas poly(allylamine) completely suppresses CO2 reduction in favor of the hydrogen evolution reaction.},
doi = {10.1021/acscatal.7b04347},
journal = {ACS Catalysis},
number = 5,
volume = 8,
place = {United States},
year = {Tue Apr 03 00:00:00 EDT 2018},
month = {Tue Apr 03 00:00:00 EDT 2018}
}
Web of Science
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