PTFE nanocoating on Cu nanoparticles through dry processing to enhance electrochemical conversion of CO2 towards multi-carbon products
Polymer modified copper (Cu) catalysts have demonstrated an increased production of multi-carbon (C2+) products during the electrochemical CO2 reduction reaction (CO2RR). Herein, a solvent-free processing method has been developed to cover commercial Cu nanoparticles with a porous nanocoating of pol...
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creator | Pellessier, John Gong, Xiangtao Li, Boyang Zhang, Jiaqi Yang, Gang Hambleton, Kirk Podder, Chinmoy Gao, Zhongjia Zhou, Hongcai Wang, Guofeng Pan, Heng Li, Ying |
description | Polymer modified copper (Cu) catalysts have demonstrated an increased production of multi-carbon (C2+) products during the electrochemical CO2 reduction reaction (CO2RR). Herein, a solvent-free processing method has been developed to cover commercial Cu nanoparticles with a porous nanocoating of polytetrafluoroethylene (PTFE) that greatly improved the production of C2+ products. The PTFE coating created a large interfacial surface area that facilitated the transport of CO2 to the solid–liquid–gas interface. The optimal catalyst achieved a faradaic efficiency of 78% for C2+ products and a notably large C2+ to C1 product ratio of ∼13 at current densities ranging from 400 to 500 mA cm−2. In comparison, catalysts prepared by a conventional solvent-based method only achieved a faradaic efficiency of 56% for C2+ products and a small C2+ to C1 product ratio of ∼2 in the same current density range. Density functional theory (DFT) calculations suggested that the physisorbed PTFE coating on Cu catalysts plays a more significant role than the most frequently studied chemisorbed PTFE. The physisorbed PTFE is predicted to increase the binding energy of CO intermediates on Cu and lower the activation energy for C–C coupling steps, leading to significantly higher C2+ product selectivity of the Cu catalysts. |
doi_str_mv | 10.1039/d3ta05787a |
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Herein, a solvent-free processing method has been developed to cover commercial Cu nanoparticles with a porous nanocoating of polytetrafluoroethylene (PTFE) that greatly improved the production of C2+ products. The PTFE coating created a large interfacial surface area that facilitated the transport of CO2 to the solid–liquid–gas interface. The optimal catalyst achieved a faradaic efficiency of 78% for C2+ products and a notably large C2+ to C1 product ratio of ∼13 at current densities ranging from 400 to 500 mA cm−2. In comparison, catalysts prepared by a conventional solvent-based method only achieved a faradaic efficiency of 56% for C2+ products and a small C2+ to C1 product ratio of ∼2 in the same current density range. Density functional theory (DFT) calculations suggested that the physisorbed PTFE coating on Cu catalysts plays a more significant role than the most frequently studied chemisorbed PTFE. The physisorbed PTFE is predicted to increase the binding energy of CO intermediates on Cu and lower the activation energy for C–C coupling steps, leading to significantly higher C2+ product selectivity of the Cu catalysts.</description><identifier>ISSN: 2050-7488</identifier><identifier>EISSN: 2050-7496</identifier><identifier>DOI: 10.1039/d3ta05787a</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Carbon dioxide ; Catalysts ; Chemical reduction ; Copper ; Copper converters ; Current density ; Density functional theory ; Electrochemistry ; Intermediates ; Nanoparticles ; Polymers ; Polytetrafluoroethylene ; Solvents</subject><ispartof>Journal of materials chemistry. A, Materials for energy and sustainability, 2023-12, Vol.11 (47), p.26252-26264</ispartof><rights>Copyright Royal Society of Chemistry 2023</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></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>Pellessier, John</creatorcontrib><creatorcontrib>Gong, Xiangtao</creatorcontrib><creatorcontrib>Li, Boyang</creatorcontrib><creatorcontrib>Zhang, Jiaqi</creatorcontrib><creatorcontrib>Yang, Gang</creatorcontrib><creatorcontrib>Hambleton, Kirk</creatorcontrib><creatorcontrib>Podder, Chinmoy</creatorcontrib><creatorcontrib>Gao, Zhongjia</creatorcontrib><creatorcontrib>Zhou, Hongcai</creatorcontrib><creatorcontrib>Wang, Guofeng</creatorcontrib><creatorcontrib>Pan, Heng</creatorcontrib><creatorcontrib>Li, Ying</creatorcontrib><title>PTFE nanocoating on Cu nanoparticles through dry processing to enhance electrochemical conversion of CO2 towards multi-carbon products</title><title>Journal of materials chemistry. A, Materials for energy and sustainability</title><description>Polymer modified copper (Cu) catalysts have demonstrated an increased production of multi-carbon (C2+) products during the electrochemical CO2 reduction reaction (CO2RR). Herein, a solvent-free processing method has been developed to cover commercial Cu nanoparticles with a porous nanocoating of polytetrafluoroethylene (PTFE) that greatly improved the production of C2+ products. The PTFE coating created a large interfacial surface area that facilitated the transport of CO2 to the solid–liquid–gas interface. The optimal catalyst achieved a faradaic efficiency of 78% for C2+ products and a notably large C2+ to C1 product ratio of ∼13 at current densities ranging from 400 to 500 mA cm−2. In comparison, catalysts prepared by a conventional solvent-based method only achieved a faradaic efficiency of 56% for C2+ products and a small C2+ to C1 product ratio of ∼2 in the same current density range. Density functional theory (DFT) calculations suggested that the physisorbed PTFE coating on Cu catalysts plays a more significant role than the most frequently studied chemisorbed PTFE. The physisorbed PTFE is predicted to increase the binding energy of CO intermediates on Cu and lower the activation energy for C–C coupling steps, leading to significantly higher C2+ product selectivity of the Cu catalysts.</description><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>Chemical reduction</subject><subject>Copper</subject><subject>Copper converters</subject><subject>Current density</subject><subject>Density functional theory</subject><subject>Electrochemistry</subject><subject>Intermediates</subject><subject>Nanoparticles</subject><subject>Polymers</subject><subject>Polytetrafluoroethylene</subject><subject>Solvents</subject><issn>2050-7488</issn><issn>2050-7496</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNo9j81OwzAQhC0EElXphSewxDlgO3FsH1HUAlKlcijnams7TarUDrYD4gV4bsyP2Muu5hvNaBG6puSWklLdmTIB4UIKOEMzRjgpRKXq8_9byku0iPFI8khCaqVm6PN5u1piB85rD6l3B-wdbqYfZYSQej3YiFMX_HTosAkfeAxe2xi_rclj6zpw2mI7WJ0y6eyp1zBg7d2bDbHPab7FzYZl8zsEE_FpGlJfaAj7zHKYmXSKV-iihSHaxd-eo5fVcts8FuvNw1Nzvy5GKstUtPlPKQTnWkDdkj2nrNZGciOhBaFVq0DQWipmDclIcSZ4TbUoeV1JQXU5Rze_ubn4dbIx7Y5-Ci5X7phUoqoqRkT5BQE2ZOA</recordid><startdate>20231205</startdate><enddate>20231205</enddate><creator>Pellessier, John</creator><creator>Gong, Xiangtao</creator><creator>Li, Boyang</creator><creator>Zhang, Jiaqi</creator><creator>Yang, Gang</creator><creator>Hambleton, Kirk</creator><creator>Podder, Chinmoy</creator><creator>Gao, Zhongjia</creator><creator>Zhou, Hongcai</creator><creator>Wang, Guofeng</creator><creator>Pan, Heng</creator><creator>Li, Ying</creator><general>Royal Society of Chemistry</general><scope>7SP</scope><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>JG9</scope><scope>L7M</scope><scope>SOI</scope></search><sort><creationdate>20231205</creationdate><title>PTFE nanocoating on Cu nanoparticles through dry processing to enhance electrochemical conversion of CO2 towards multi-carbon products</title><author>Pellessier, John ; Gong, Xiangtao ; Li, Boyang ; Zhang, Jiaqi ; Yang, Gang ; Hambleton, Kirk ; Podder, Chinmoy ; Gao, Zhongjia ; Zhou, Hongcai ; Wang, Guofeng ; Pan, Heng ; Li, Ying</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p183t-f10387755c7a6f0b5126cd85d8afa7c9f9a716892ed01269527561c73564871c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>Chemical reduction</topic><topic>Copper</topic><topic>Copper converters</topic><topic>Current density</topic><topic>Density functional theory</topic><topic>Electrochemistry</topic><topic>Intermediates</topic><topic>Nanoparticles</topic><topic>Polymers</topic><topic>Polytetrafluoroethylene</topic><topic>Solvents</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Pellessier, John</creatorcontrib><creatorcontrib>Gong, Xiangtao</creatorcontrib><creatorcontrib>Li, Boyang</creatorcontrib><creatorcontrib>Zhang, Jiaqi</creatorcontrib><creatorcontrib>Yang, Gang</creatorcontrib><creatorcontrib>Hambleton, Kirk</creatorcontrib><creatorcontrib>Podder, Chinmoy</creatorcontrib><creatorcontrib>Gao, Zhongjia</creatorcontrib><creatorcontrib>Zhou, Hongcai</creatorcontrib><creatorcontrib>Wang, Guofeng</creatorcontrib><creatorcontrib>Pan, Heng</creatorcontrib><creatorcontrib>Li, Ying</creatorcontrib><collection>Electronics & Communications Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Journal of materials chemistry. A, Materials for energy and sustainability</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Pellessier, John</au><au>Gong, Xiangtao</au><au>Li, Boyang</au><au>Zhang, Jiaqi</au><au>Yang, Gang</au><au>Hambleton, Kirk</au><au>Podder, Chinmoy</au><au>Gao, Zhongjia</au><au>Zhou, Hongcai</au><au>Wang, Guofeng</au><au>Pan, Heng</au><au>Li, Ying</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>PTFE nanocoating on Cu nanoparticles through dry processing to enhance electrochemical conversion of CO2 towards multi-carbon products</atitle><jtitle>Journal of materials chemistry. A, Materials for energy and sustainability</jtitle><date>2023-12-05</date><risdate>2023</risdate><volume>11</volume><issue>47</issue><spage>26252</spage><epage>26264</epage><pages>26252-26264</pages><issn>2050-7488</issn><eissn>2050-7496</eissn><abstract>Polymer modified copper (Cu) catalysts have demonstrated an increased production of multi-carbon (C2+) products during the electrochemical CO2 reduction reaction (CO2RR). Herein, a solvent-free processing method has been developed to cover commercial Cu nanoparticles with a porous nanocoating of polytetrafluoroethylene (PTFE) that greatly improved the production of C2+ products. The PTFE coating created a large interfacial surface area that facilitated the transport of CO2 to the solid–liquid–gas interface. The optimal catalyst achieved a faradaic efficiency of 78% for C2+ products and a notably large C2+ to C1 product ratio of ∼13 at current densities ranging from 400 to 500 mA cm−2. In comparison, catalysts prepared by a conventional solvent-based method only achieved a faradaic efficiency of 56% for C2+ products and a small C2+ to C1 product ratio of ∼2 in the same current density range. Density functional theory (DFT) calculations suggested that the physisorbed PTFE coating on Cu catalysts plays a more significant role than the most frequently studied chemisorbed PTFE. The physisorbed PTFE is predicted to increase the binding energy of CO intermediates on Cu and lower the activation energy for C–C coupling steps, leading to significantly higher C2+ product selectivity of the Cu catalysts.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d3ta05787a</doi><tpages>13</tpages></addata></record> |
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subjects | Carbon dioxide Catalysts Chemical reduction Copper Copper converters Current density Density functional theory Electrochemistry Intermediates Nanoparticles Polymers Polytetrafluoroethylene Solvents |
title | PTFE nanocoating on Cu nanoparticles through dry processing to enhance electrochemical conversion of CO2 towards multi-carbon products |
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