Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide

Ahn, Sunyhik; Klyukin, Konstantin; Wakeham, Russell J.; Rudd, Jennifer A.; Lewis, Aled R.; Alexander, Shirin; Carla, Francesco; Alexandrov, Vitaly; Andreoli, Enrico

doi:10.1021/acscatal.7b04347

Title: Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide

Journal Article · 03 April 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.7b04347 · OSTI ID:1543699

Ahn, Sunyhik ^[1];

^[2];

^[1]; Rudd, Jennifer A. ^[1]; Lewis, Aled R. ^[1];

^[1]; Carla, Francesco ^[3]; Alexandrov, Vitaly ^[2];

^[1]

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)

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1543699

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 5 Vol. 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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