CO residence time modulates multi-carbon formation rates in a zero-gap Cu based CO 2 electrolyzer
Carbon dioxide (CO 2 ) electrolysis on copper (Cu) catalysts has attracted interest due to its direct production of C 2+ feedstocks. Using the knowledge that CO 2 reduction on copper is primarily a tandem reaction of CO 2 to CO and CO to C 2+ products, we show that modulating CO concentrations withi...
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| Veröffentlicht in: | Energy & environmental science 2024-09, Vol.17 (18), p.6728-6738 |
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| creator | Subramanian, Siddhartha Kok, Jesse Gholkar, Pratik Sajeev Kumar, Asvin Iglesias van Montfort, Hugo-Pieter Kortlever, Ruud Urakawa, Atsushi Dam, Bernard Burdyny, Thomas |
| description | Carbon dioxide (CO
2
) electrolysis on copper (Cu) catalysts has attracted interest due to its direct production of C
2+
feedstocks. Using the knowledge that CO
2
reduction on copper is primarily a tandem reaction of CO
2
to CO and CO to C
2+
products, we show that modulating CO concentrations within the liquid catalyst layer allows for a C
2+
selectivity of >80% at 200 mA cm
−2
under broad conversion conditions. The importance of CO pooling is demonstrated through residence time distribution curves, varying flow fields (serpentine/parallel/interdigitated), and flow rates. While serpentine flow fields require high conversions to limit CO selectivity and maximize C
2+
selectivity, the longer CO residence times of parallel flow fields achieve similar selectivity over broad flow rates. Critically, we show that parts of the catalyst area predominantly reduce CO instead of CO
2
as supported by CO reduction experiments, transport modelling, and achieving a CO
2
utilization efficiency greater than the theoretical limit of 25% for C
2+
products. |
| doi_str_mv | 10.1039/D4EE02004A |
| format | Article |
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2
) electrolysis on copper (Cu) catalysts has attracted interest due to its direct production of C
2+
feedstocks. Using the knowledge that CO
2
reduction on copper is primarily a tandem reaction of CO
2
to CO and CO to C
2+
products, we show that modulating CO concentrations within the liquid catalyst layer allows for a C
2+
selectivity of >80% at 200 mA cm
−2
under broad conversion conditions. The importance of CO pooling is demonstrated through residence time distribution curves, varying flow fields (serpentine/parallel/interdigitated), and flow rates. While serpentine flow fields require high conversions to limit CO selectivity and maximize C
2+
selectivity, the longer CO residence times of parallel flow fields achieve similar selectivity over broad flow rates. Critically, we show that parts of the catalyst area predominantly reduce CO instead of CO
2
as supported by CO reduction experiments, transport modelling, and achieving a CO
2
utilization efficiency greater than the theoretical limit of 25% for C
2+
products.</description><identifier>ISSN: 1754-5692</identifier><identifier>EISSN: 1754-5706</identifier><identifier>DOI: 10.1039/D4EE02004A</identifier><language>eng</language><ispartof>Energy & environmental science, 2024-09, Vol.17 (18), p.6728-6738</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-crossref_primary_10_1039_D4EE02004A3</cites><orcidid>0000-0002-7992-3849 ; 0000-0002-8584-7336 ; 0000-0001-8057-9558 ; 0000-0001-9412-7480 ; 0000-0001-7778-4008 ; 0000-0001-6791-7292 ; 0000-0002-9594-392X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids></links><search><creatorcontrib>Subramanian, Siddhartha</creatorcontrib><creatorcontrib>Kok, Jesse</creatorcontrib><creatorcontrib>Gholkar, Pratik</creatorcontrib><creatorcontrib>Sajeev Kumar, Asvin</creatorcontrib><creatorcontrib>Iglesias van Montfort, Hugo-Pieter</creatorcontrib><creatorcontrib>Kortlever, Ruud</creatorcontrib><creatorcontrib>Urakawa, Atsushi</creatorcontrib><creatorcontrib>Dam, Bernard</creatorcontrib><creatorcontrib>Burdyny, Thomas</creatorcontrib><title>CO residence time modulates multi-carbon formation rates in a zero-gap Cu based CO 2 electrolyzer</title><title>Energy & environmental science</title><description>Carbon dioxide (CO
2
) electrolysis on copper (Cu) catalysts has attracted interest due to its direct production of C
2+
feedstocks. Using the knowledge that CO
2
reduction on copper is primarily a tandem reaction of CO
2
to CO and CO to C
2+
products, we show that modulating CO concentrations within the liquid catalyst layer allows for a C
2+
selectivity of >80% at 200 mA cm
−2
under broad conversion conditions. The importance of CO pooling is demonstrated through residence time distribution curves, varying flow fields (serpentine/parallel/interdigitated), and flow rates. While serpentine flow fields require high conversions to limit CO selectivity and maximize C
2+
selectivity, the longer CO residence times of parallel flow fields achieve similar selectivity over broad flow rates. Critically, we show that parts of the catalyst area predominantly reduce CO instead of CO
2
as supported by CO reduction experiments, transport modelling, and achieving a CO
2
utilization efficiency greater than the theoretical limit of 25% for C
2+
products.</description><issn>1754-5692</issn><issn>1754-5706</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqVj0FrwkAQhZeiUK299BfMWYidxJiQY0kj3nrpPYzJRFZ2szK7OdhfbyqKZ0_vg_d48Cn1EeMqxnXx-Z1WFSaI6deLmsX5Jo02OWaTO2dF8qrm3h8RswTzYqao_AFhr1vuG4agLYN17WAosAc7mKCjhmTveuicWAp6JLmWugeCPxYXHegE5QB78tzC-JcAG26COHMe-4WadmQ8v9_yTS231W-5ixpx3gt39Um0JTnXMdb_EvVDYv3U-AKZA0zS</recordid><startdate>20240918</startdate><enddate>20240918</enddate><creator>Subramanian, Siddhartha</creator><creator>Kok, Jesse</creator><creator>Gholkar, Pratik</creator><creator>Sajeev Kumar, Asvin</creator><creator>Iglesias van Montfort, Hugo-Pieter</creator><creator>Kortlever, Ruud</creator><creator>Urakawa, Atsushi</creator><creator>Dam, Bernard</creator><creator>Burdyny, Thomas</creator><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-7992-3849</orcidid><orcidid>https://orcid.org/0000-0002-8584-7336</orcidid><orcidid>https://orcid.org/0000-0001-8057-9558</orcidid><orcidid>https://orcid.org/0000-0001-9412-7480</orcidid><orcidid>https://orcid.org/0000-0001-7778-4008</orcidid><orcidid>https://orcid.org/0000-0001-6791-7292</orcidid><orcidid>https://orcid.org/0000-0002-9594-392X</orcidid></search><sort><creationdate>20240918</creationdate><title>CO residence time modulates multi-carbon formation rates in a zero-gap Cu based CO 2 electrolyzer</title><author>Subramanian, Siddhartha ; Kok, Jesse ; Gholkar, Pratik ; Sajeev Kumar, Asvin ; Iglesias van Montfort, Hugo-Pieter ; Kortlever, Ruud ; Urakawa, Atsushi ; Dam, Bernard ; Burdyny, Thomas</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-crossref_primary_10_1039_D4EE02004A3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Subramanian, Siddhartha</creatorcontrib><creatorcontrib>Kok, Jesse</creatorcontrib><creatorcontrib>Gholkar, Pratik</creatorcontrib><creatorcontrib>Sajeev Kumar, Asvin</creatorcontrib><creatorcontrib>Iglesias van Montfort, Hugo-Pieter</creatorcontrib><creatorcontrib>Kortlever, Ruud</creatorcontrib><creatorcontrib>Urakawa, Atsushi</creatorcontrib><creatorcontrib>Dam, Bernard</creatorcontrib><creatorcontrib>Burdyny, Thomas</creatorcontrib><collection>CrossRef</collection><jtitle>Energy & environmental science</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Subramanian, Siddhartha</au><au>Kok, Jesse</au><au>Gholkar, Pratik</au><au>Sajeev Kumar, Asvin</au><au>Iglesias van Montfort, Hugo-Pieter</au><au>Kortlever, Ruud</au><au>Urakawa, Atsushi</au><au>Dam, Bernard</au><au>Burdyny, Thomas</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>CO residence time modulates multi-carbon formation rates in a zero-gap Cu based CO 2 electrolyzer</atitle><jtitle>Energy & environmental science</jtitle><date>2024-09-18</date><risdate>2024</risdate><volume>17</volume><issue>18</issue><spage>6728</spage><epage>6738</epage><pages>6728-6738</pages><issn>1754-5692</issn><eissn>1754-5706</eissn><abstract>Carbon dioxide (CO
2
) electrolysis on copper (Cu) catalysts has attracted interest due to its direct production of C
2+
feedstocks. Using the knowledge that CO
2
reduction on copper is primarily a tandem reaction of CO
2
to CO and CO to C
2+
products, we show that modulating CO concentrations within the liquid catalyst layer allows for a C
2+
selectivity of >80% at 200 mA cm
−2
under broad conversion conditions. The importance of CO pooling is demonstrated through residence time distribution curves, varying flow fields (serpentine/parallel/interdigitated), and flow rates. While serpentine flow fields require high conversions to limit CO selectivity and maximize C
2+
selectivity, the longer CO residence times of parallel flow fields achieve similar selectivity over broad flow rates. Critically, we show that parts of the catalyst area predominantly reduce CO instead of CO
2
as supported by CO reduction experiments, transport modelling, and achieving a CO
2
utilization efficiency greater than the theoretical limit of 25% for C
2+
products.</abstract><doi>10.1039/D4EE02004A</doi><orcidid>https://orcid.org/0000-0002-7992-3849</orcidid><orcidid>https://orcid.org/0000-0002-8584-7336</orcidid><orcidid>https://orcid.org/0000-0001-8057-9558</orcidid><orcidid>https://orcid.org/0000-0001-9412-7480</orcidid><orcidid>https://orcid.org/0000-0001-7778-4008</orcidid><orcidid>https://orcid.org/0000-0001-6791-7292</orcidid><orcidid>https://orcid.org/0000-0002-9594-392X</orcidid></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 1754-5692 |
| ispartof | Energy & environmental science, 2024-09, Vol.17 (18), p.6728-6738 |
| issn | 1754-5692 1754-5706 |
| language | eng |
| recordid | cdi_crossref_primary_10_1039_D4EE02004A |
| source | Royal Society Of Chemistry Journals 2008- |
| title | CO residence time modulates multi-carbon formation rates in a zero-gap Cu based CO 2 electrolyzer |
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