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Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide / Sunyhik Ahn, Konstantin Klyukin, Russell Wakeham, Jennifer Rudd, Aled R. Lewis, Shirin Alexander, Francesco Carla, Vitaly Alexandrov, Enrico Andreoli

ACS Catalysis, Volume: 8, Issue: 5, Pages: 4132 - 4142

Swansea University Authors: Russell Wakeham, Jennifer Rudd, Shirin Alexander, Enrico Andreoli

Abstract

A new strategy to modulate the electrocatalytic activity of copper towards 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...

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Published in: ACS Catalysis
ISSN: 2155-5435 2155-5435
Published: 2018
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URI: https://cronfa.swan.ac.uk/Record/cronfa39347
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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 multi-point binding catalytic system where the interplay between activation and stabilization of intermediates results in enhanced selectivity toward ethylene formation. 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.</abstract><type>Journal Article</type><journal>ACS Catalysis</journal><volume>8</volume><journalNumber>5</journalNumber><paginationStart>4132</paginationStart><paginationEnd>4142</paginationEnd><publisher/><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>2155-5435</issnPrint><issnElectronic>2155-5435</issnElectronic><keywords/><publishedDay>31</publishedDay><publishedMonth>12</publishedMonth><publishedYear>2018</publishedYear><publishedDate>2018-12-31</publishedDate><doi>10.1021/acscatal.7b04347</doi><url/><notes/><college>COLLEGE NANME</college><department>Engineering</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>EEN</DepartmentCode><institution>Swansea University</institution><apcterm/><lastEdited>2020-12-09T15:41:52.4308090</lastEdited><Created>2018-04-09T12:02:08.3708728</Created><path><level id="1"/><level id="2"/></path><authors><author><firstname>Sunyhik</firstname><surname>Ahn</surname><order>1</order></author><author><firstname>Konstantin</firstname><surname>Klyukin</surname><order>2</order></author><author><firstname>Russell</firstname><surname>Wakeham</surname><orcid>0000-0002-4304-0243</orcid><order>3</order></author><author><firstname>Jennifer</firstname><surname>Rudd</surname><orcid>0000-0002-5209-477X</orcid><order>4</order></author><author><firstname>Aled R.</firstname><surname>Lewis</surname><order>5</order></author><author><firstname>Shirin</firstname><surname>Alexander</surname><orcid>0000-0002-4404-0026</orcid><order>6</order></author><author><firstname>Francesco</firstname><surname>Carla</surname><order>7</order></author><author><firstname>Vitaly</firstname><surname>Alexandrov</surname><order>8</order></author><author><firstname>Enrico</firstname><surname>Andreoli</surname><orcid>0000-0002-1207-2314</orcid><order>9</order></author></authors><documents><document><filename>0039347-09042018120421.pdf</filename><originalFilename>ahn2018.pdf</originalFilename><uploaded>2018-04-09T12:04:21.4870000</uploaded><type>Output</type><contentLength>10490126</contentLength><contentType>application/pdf</contentType><version>Accepted Manuscript</version><cronfaStatus>true</cronfaStatus><action/><embargoDate>2019-04-03T00:00:00.0000000</embargoDate><copyrightCorrect>true</copyrightCorrect><language>eng</language></document></documents><OutputDurs/></rfc1807>
spelling 2020-12-09T15:41:52.4308090 v2 39347 2018-04-09 Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide 28c45bbeeba294da7042950705b98e0a 0000-0002-4304-0243 Russell Wakeham Russell Wakeham true false c2e4cf0f048a86b5ca2f331e6c566aff 0000-0002-5209-477X Jennifer Rudd Jennifer Rudd true false 0773cc55f7caf77817be08806b8b7497 0000-0002-4404-0026 Shirin Alexander Shirin Alexander true false cbd843daab780bb55698a3daccd74df8 0000-0002-1207-2314 Enrico Andreoli Enrico Andreoli true false 2018-04-09 EEN A new strategy to modulate the electrocatalytic activity of copper towards 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 multi-point binding catalytic system where the interplay between activation and stabilization of intermediates results in enhanced selectivity toward ethylene formation. 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. Journal Article ACS Catalysis 8 5 4132 4142 2155-5435 2155-5435 31 12 2018 2018-12-31 10.1021/acscatal.7b04347 COLLEGE NANME Engineering COLLEGE CODE EEN Swansea University 2020-12-09T15:41:52.4308090 2018-04-09T12:02:08.3708728 Sunyhik Ahn 1 Konstantin Klyukin 2 Russell Wakeham 0000-0002-4304-0243 3 Jennifer Rudd 0000-0002-5209-477X 4 Aled R. Lewis 5 Shirin Alexander 0000-0002-4404-0026 6 Francesco Carla 7 Vitaly Alexandrov 8 Enrico Andreoli 0000-0002-1207-2314 9 0039347-09042018120421.pdf ahn2018.pdf 2018-04-09T12:04:21.4870000 Output 10490126 application/pdf Accepted Manuscript true 2019-04-03T00:00:00.0000000 true eng
title Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
spellingShingle Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
Russell, Wakeham
Jennifer, Rudd
Shirin, Alexander
Enrico, Andreoli
title_short Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
title_full Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
title_fullStr Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
title_full_unstemmed Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
title_sort Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
author_id_str_mv 28c45bbeeba294da7042950705b98e0a
c2e4cf0f048a86b5ca2f331e6c566aff
0773cc55f7caf77817be08806b8b7497
cbd843daab780bb55698a3daccd74df8
author_id_fullname_str_mv 28c45bbeeba294da7042950705b98e0a_***_Russell, Wakeham
c2e4cf0f048a86b5ca2f331e6c566aff_***_Jennifer, Rudd
0773cc55f7caf77817be08806b8b7497_***_Shirin, Alexander
cbd843daab780bb55698a3daccd74df8_***_Enrico, Andreoli
author Russell, Wakeham
Jennifer, Rudd
Shirin, Alexander
Enrico, Andreoli
author2 Sunyhik Ahn
Konstantin Klyukin
Russell Wakeham
Jennifer Rudd
Aled R. Lewis
Shirin Alexander
Francesco Carla
Vitaly Alexandrov
Enrico Andreoli
format Journal article
container_title ACS Catalysis
container_volume 8
container_issue 5
container_start_page 4132
publishDate 2018
institution Swansea University
issn 2155-5435
2155-5435
doi_str_mv 10.1021/acscatal.7b04347
document_store_str 1
active_str 0
description A new strategy to modulate the electrocatalytic activity of copper towards 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 multi-point binding catalytic system where the interplay between activation and stabilization of intermediates results in enhanced selectivity toward ethylene formation. 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.
published_date 2018-12-31T03:58:19Z
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