Journal article 1520 views 948 downloads
Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide
ACS Catalysis, Volume: 8, Issue: 5, Pages: 4132 - 4142
Swansea University Authors: Russell Wakeham , Jennifer Rudd , Shirin Alexander , Enrico Andreoli
-
PDF | Accepted Manuscript
Download (10.04MB)
DOI (Published version): 10.1021/acscatal.7b04347
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...
Published in: | ACS Catalysis |
---|---|
ISSN: | 2155-5435 2155-5435 |
Published: |
2018
|
Online Access: |
Check full text
|
URI: | https://cronfa.swan.ac.uk/Record/cronfa39347 |
Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
first_indexed |
2018-04-09T13:29:58Z |
---|---|
last_indexed |
2023-02-15T03:48:25Z |
id |
cronfa39347 |
recordtype |
SURis |
fullrecord |
<?xml version="1.0"?><rfc1807><datestamp>2023-02-14T15:27:30.6352198</datestamp><bib-version>v2</bib-version><id>39347</id><entry>2018-04-09</entry><title>Poly-Amide Modified Copper Foam Electrodes for Enhanced Electrochemical Reduction of Carbon Dioxide</title><swanseaauthors><author><sid>28c45bbeeba294da7042950705b98e0a</sid><ORCID>0000-0002-4304-0243</ORCID><firstname>Russell</firstname><surname>Wakeham</surname><name>Russell Wakeham</name><active>true</active><ethesisStudent>false</ethesisStudent></author><author><sid>c2e4cf0f048a86b5ca2f331e6c566aff</sid><ORCID>0000-0002-5209-477X</ORCID><firstname>Jennifer</firstname><surname>Rudd</surname><name>Jennifer Rudd</name><active>true</active><ethesisStudent>false</ethesisStudent></author><author><sid>0773cc55f7caf77817be08806b8b7497</sid><ORCID>0000-0002-4404-0026</ORCID><firstname>Shirin</firstname><surname>Alexander</surname><name>Shirin Alexander</name><active>true</active><ethesisStudent>false</ethesisStudent></author><author><sid>cbd843daab780bb55698a3daccd74df8</sid><ORCID>0000-0002-1207-2314</ORCID><firstname>Enrico</firstname><surname>Andreoli</surname><name>Enrico Andreoli</name><active>true</active><ethesisStudent>false</ethesisStudent></author></swanseaauthors><date>2018-04-09</date><deptcode>EEN</deptcode><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 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/><funders/><projectreference/><lastEdited>2023-02-14T15:27:30.6352198</lastEdited><Created>2018-04-09T12:02:08.3708728</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Chemical Engineering</level></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><embargoDate>2019-04-03T00:00:00.0000000</embargoDate><copyrightCorrect>true</copyrightCorrect><language>eng</language></document></documents><OutputDurs/></rfc1807> |
spelling |
2023-02-14T15:27:30.6352198 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 2023-02-14T15:27:30.6352198 2018-04-09T12:02:08.3708728 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering 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 |
college_str |
Faculty of Science and Engineering |
hierarchytype |
|
hierarchy_top_id |
facultyofscienceandengineering |
hierarchy_top_title |
Faculty of Science and Engineering |
hierarchy_parent_id |
facultyofscienceandengineering |
hierarchy_parent_title |
Faculty of Science and Engineering |
department_str |
School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering |
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 |
2018-12-31T03:49:57Z |
_version_ |
1763752435031998464 |
score |
11.013148 |