Electrochemical Flow Reactor Design Allows Tunable Mass Transport Conditions for Operando Surface Enhanced Infrared Absorption Spectroscopy
In situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR‐SEIRAS) is often used to investigate the near‐surface electrocatalytic reaction environment. However, there is a gap in directly correlating the near‐surface reaction environment with electrocatalytic reaction...
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| creator | Avilés Acosta, Jaime E. Lin, John C. Un Lee, Dong Jaramillo, Thomas F. Hahn, Christopher |
| description | In situ
attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR‐SEIRAS) is often used to investigate the near‐surface electrocatalytic reaction environment. However, there is a gap in directly correlating the near‐surface reaction environment with electrocatalytic reaction rates. To that end, we designed an electrochemical flow reactor for
operando
electrochemical ATR‐SEIRAS and demonstrate its capability with the CO
2
reduction reaction (CO
2
RR). Roughened gold catalyst thin films are prepared on ATR silicon crystals as a model system to probe local species under CO
2
RR conditions in 0.1 M KHCO
3
. We measured changes in the interfacial CO
2
concentration as a function of applied potential and electrolyte flow rate in
operando
, allowing us to correlate the changes in reaction rates with the observed CO
2
concentration. Including the choice of the catalyst and electrolyte, coupling hydrodynamic control with ATR‐SEIRAS in this platform enables investigations of how the local microenvironment affects the activity and selectivity of electrochemical reactions. |
| doi_str_mv | 10.1002/cctc.202300520 |
| format | Article |
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attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR‐SEIRAS) is often used to investigate the near‐surface electrocatalytic reaction environment. However, there is a gap in directly correlating the near‐surface reaction environment with electrocatalytic reaction rates. To that end, we designed an electrochemical flow reactor for
operando
electrochemical ATR‐SEIRAS and demonstrate its capability with the CO
2
reduction reaction (CO
2
RR). Roughened gold catalyst thin films are prepared on ATR silicon crystals as a model system to probe local species under CO
2
RR conditions in 0.1 M KHCO
3
. We measured changes in the interfacial CO
2
concentration as a function of applied potential and electrolyte flow rate in
operando
, allowing us to correlate the changes in reaction rates with the observed CO
2
concentration. Including the choice of the catalyst and electrolyte, coupling hydrodynamic control with ATR‐SEIRAS in this platform enables investigations of how the local microenvironment affects the activity and selectivity of electrochemical reactions.</description><identifier>ISSN: 1867-3880</identifier><identifier>EISSN: 1867-3899</identifier><identifier>DOI: 10.1002/cctc.202300520</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Absorption spectroscopy ; Carbon dioxide ; Carbon dioxide concentration ; Catalysts ; Chemical reactions ; Chemical reduction ; Infrared absorption ; Infrared reflection ; Infrared spectroscopy ; Mass transport ; Reactor design ; Surface chemistry ; Surface reactions ; Thin films</subject><ispartof>ChemCatChem, 2023-08, Vol.15 (15)</ispartof><rights>2023 Wiley‐VCH Verlag GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c294t-c251c6cf7f1936598f882ac9ee0105d001948a8be049744fc5182961c0d124203</citedby><cites>FETCH-LOGICAL-c294t-c251c6cf7f1936598f882ac9ee0105d001948a8be049744fc5182961c0d124203</cites><orcidid>0000-0001-7591-5350 ; 0000-0002-2259-1935 ; 0000-0001-9900-0622 ; 0000-0002-2772-6341 ; 0000000175915350 ; 0000000227726341 ; 0000000199000622 ; 0000000222591935</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,315,781,785,886,27926,27927</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1994586$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Avilés Acosta, Jaime E.</creatorcontrib><creatorcontrib>Lin, John C.</creatorcontrib><creatorcontrib>Un Lee, Dong</creatorcontrib><creatorcontrib>Jaramillo, Thomas F.</creatorcontrib><creatorcontrib>Hahn, Christopher</creatorcontrib><title>Electrochemical Flow Reactor Design Allows Tunable Mass Transport Conditions for Operando Surface Enhanced Infrared Absorption Spectroscopy</title><title>ChemCatChem</title><description>In situ
attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR‐SEIRAS) is often used to investigate the near‐surface electrocatalytic reaction environment. However, there is a gap in directly correlating the near‐surface reaction environment with electrocatalytic reaction rates. To that end, we designed an electrochemical flow reactor for
operando
electrochemical ATR‐SEIRAS and demonstrate its capability with the CO
2
reduction reaction (CO
2
RR). Roughened gold catalyst thin films are prepared on ATR silicon crystals as a model system to probe local species under CO
2
RR conditions in 0.1 M KHCO
3
. We measured changes in the interfacial CO
2
concentration as a function of applied potential and electrolyte flow rate in
operando
, allowing us to correlate the changes in reaction rates with the observed CO
2
concentration. Including the choice of the catalyst and electrolyte, coupling hydrodynamic control with ATR‐SEIRAS in this platform enables investigations of how the local microenvironment affects the activity and selectivity of electrochemical reactions.</description><subject>Absorption spectroscopy</subject><subject>Carbon dioxide</subject><subject>Carbon dioxide concentration</subject><subject>Catalysts</subject><subject>Chemical reactions</subject><subject>Chemical reduction</subject><subject>Infrared absorption</subject><subject>Infrared reflection</subject><subject>Infrared spectroscopy</subject><subject>Mass transport</subject><subject>Reactor design</subject><subject>Surface chemistry</subject><subject>Surface reactions</subject><subject>Thin films</subject><issn>1867-3880</issn><issn>1867-3899</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNo9UclOwzAQjRBIlOXK2YJzy9hxEvtYlQKVQEgsZ8ud2DRVagfbFeIb-GlcirjM-t4sekVxQWFCAdg1YsIJA1YCVAwOihEVdTMuhZSH_7GA4-IkxjVALcumGhXf895gCh5XZtOh7slt7z_Js9GYfCA3Jnbvjkz7XIzkdev0sjfkUcecBO3i4EMiM-_aLnXeRWIz52kwudV68rINVqMhc7fSDk1LFs4GHXIwXUYfhh2FvAy_6yP64eusOLK6j-b8z58Wb7fz19n9-OHpbjGbPoyRSZ6yrSjWaBtLZVlXUlghmEZpDFCoWgAqudBiaYDLhnOLFRVM1hShpYwzKE-Ly_1cH1OnInbJ4Aq9c_kURaXklagz6GoPGoL_2JqY1Npvg8t3KSa4ANpUvMmoyR6F-YcYjFVD6DY6fCkKaqeK2qmi_lUpfwCWWYE2</recordid><startdate>20230807</startdate><enddate>20230807</enddate><creator>Avilés Acosta, Jaime E.</creator><creator>Lin, John C.</creator><creator>Un Lee, Dong</creator><creator>Jaramillo, Thomas F.</creator><creator>Hahn, Christopher</creator><general>Wiley Subscription Services, Inc</general><general>Wiley Blackwell (John Wiley & Sons)</general><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-7591-5350</orcidid><orcidid>https://orcid.org/0000-0002-2259-1935</orcidid><orcidid>https://orcid.org/0000-0001-9900-0622</orcidid><orcidid>https://orcid.org/0000-0002-2772-6341</orcidid><orcidid>https://orcid.org/0000000175915350</orcidid><orcidid>https://orcid.org/0000000227726341</orcidid><orcidid>https://orcid.org/0000000199000622</orcidid><orcidid>https://orcid.org/0000000222591935</orcidid></search><sort><creationdate>20230807</creationdate><title>Electrochemical Flow Reactor Design Allows Tunable Mass Transport Conditions for Operando Surface Enhanced Infrared Absorption Spectroscopy</title><author>Avilés Acosta, Jaime E. ; Lin, John C. ; Un Lee, Dong ; Jaramillo, Thomas F. ; Hahn, Christopher</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c294t-c251c6cf7f1936598f882ac9ee0105d001948a8be049744fc5182961c0d124203</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Absorption spectroscopy</topic><topic>Carbon dioxide</topic><topic>Carbon dioxide concentration</topic><topic>Catalysts</topic><topic>Chemical reactions</topic><topic>Chemical reduction</topic><topic>Infrared absorption</topic><topic>Infrared reflection</topic><topic>Infrared spectroscopy</topic><topic>Mass transport</topic><topic>Reactor design</topic><topic>Surface chemistry</topic><topic>Surface reactions</topic><topic>Thin films</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Avilés Acosta, Jaime E.</creatorcontrib><creatorcontrib>Lin, John C.</creatorcontrib><creatorcontrib>Un Lee, Dong</creatorcontrib><creatorcontrib>Jaramillo, Thomas F.</creatorcontrib><creatorcontrib>Hahn, Christopher</creatorcontrib><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>ChemCatChem</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Avilés Acosta, Jaime E.</au><au>Lin, John C.</au><au>Un Lee, Dong</au><au>Jaramillo, Thomas F.</au><au>Hahn, Christopher</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Electrochemical Flow Reactor Design Allows Tunable Mass Transport Conditions for Operando Surface Enhanced Infrared Absorption Spectroscopy</atitle><jtitle>ChemCatChem</jtitle><date>2023-08-07</date><risdate>2023</risdate><volume>15</volume><issue>15</issue><issn>1867-3880</issn><eissn>1867-3899</eissn><abstract>In situ
attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR‐SEIRAS) is often used to investigate the near‐surface electrocatalytic reaction environment. However, there is a gap in directly correlating the near‐surface reaction environment with electrocatalytic reaction rates. To that end, we designed an electrochemical flow reactor for
operando
electrochemical ATR‐SEIRAS and demonstrate its capability with the CO
2
reduction reaction (CO
2
RR). Roughened gold catalyst thin films are prepared on ATR silicon crystals as a model system to probe local species under CO
2
RR conditions in 0.1 M KHCO
3
. We measured changes in the interfacial CO
2
concentration as a function of applied potential and electrolyte flow rate in
operando
, allowing us to correlate the changes in reaction rates with the observed CO
2
concentration. Including the choice of the catalyst and electrolyte, coupling hydrodynamic control with ATR‐SEIRAS in this platform enables investigations of how the local microenvironment affects the activity and selectivity of electrochemical reactions.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/cctc.202300520</doi><orcidid>https://orcid.org/0000-0001-7591-5350</orcidid><orcidid>https://orcid.org/0000-0002-2259-1935</orcidid><orcidid>https://orcid.org/0000-0001-9900-0622</orcidid><orcidid>https://orcid.org/0000-0002-2772-6341</orcidid><orcidid>https://orcid.org/0000000175915350</orcidid><orcidid>https://orcid.org/0000000227726341</orcidid><orcidid>https://orcid.org/0000000199000622</orcidid><orcidid>https://orcid.org/0000000222591935</orcidid></addata></record> |
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| subjects | Absorption spectroscopy Carbon dioxide Carbon dioxide concentration Catalysts Chemical reactions Chemical reduction Infrared absorption Infrared reflection Infrared spectroscopy Mass transport Reactor design Surface chemistry Surface reactions Thin films |
| title | Electrochemical Flow Reactor Design Allows Tunable Mass Transport Conditions for Operando Surface Enhanced Infrared Absorption Spectroscopy |
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