Toward High‐Performance CO2‐to‐C2 Electroreduction via Linker Tuning on MOF‐Derived Catalysts
Copper (Cu)‐based metal–organic frameworks (MOFs) and MOF‐derived catalysts are well studied for electroreduction of carbon dioxide (CO2); however, the effects of organic linkers for the selectivity of CO2 reduction are still unrevealed. Here, a series of Cu‐based MOF‐derived catalysts is investigat...
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| Veröffentlicht in: | Small (Weinheim an der Bergstrasse, Germany) Germany), 2022-05, Vol.18 (18), p.e2200720-n/a |
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| creator | Chen, Rongzhen Cheng, Ling Liu, Jinze Wang, Yating Ge, Wangxin Xiao, Chuqian Jiang, Hao Li, Yuhang Li, Chunzhong |
| description | Copper (Cu)‐based metal–organic frameworks (MOFs) and MOF‐derived catalysts are well studied for electroreduction of carbon dioxide (CO2); however, the effects of organic linkers for the selectivity of CO2 reduction are still unrevealed. Here, a series of Cu‐based MOF‐derived catalysts is investigated with different organic linkers appended, named X‐Cu‐BDC (BDC = 1,4‐benzenedicarboxylic acid, X = NH2, OH, H, F, and 2F). It is found that the linkers affect the faradaic efficiency (FE) for C2 products with an order of NH2 |
| doi_str_mv | 10.1002/smll.202200720 |
| format | Article |
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The organic linker effects on Cu‐1,4‐benzene dicarboxylate metal–organic frameworks derived catalysts enable electrocatalytic CO2 reduction to multicarbon products including ethylene, ethanol with a total C2 faradaic efficiency of about 63% at a current density of 150 mA cm−2.</description><identifier>ISSN: 1613-6810</identifier><identifier>EISSN: 1613-6829</identifier><identifier>DOI: 10.1002/smll.202200720</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>C 2 products ; Carbon dioxide ; Catalysts ; CO 2 electroreduction ; Copper ; Cu metal–organic frameworks ; Electrowinning ; Fluorine ; Metal-organic frameworks ; Nanotechnology ; organic linkers ; Selectivity ; Tuning</subject><ispartof>Small (Weinheim an der Bergstrasse, Germany), 2022-05, Vol.18 (18), p.e2200720-n/a</ispartof><rights>2022 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0001-7897-5850</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fsmll.202200720$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fsmll.202200720$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids></links><search><creatorcontrib>Chen, Rongzhen</creatorcontrib><creatorcontrib>Cheng, Ling</creatorcontrib><creatorcontrib>Liu, Jinze</creatorcontrib><creatorcontrib>Wang, Yating</creatorcontrib><creatorcontrib>Ge, Wangxin</creatorcontrib><creatorcontrib>Xiao, Chuqian</creatorcontrib><creatorcontrib>Jiang, Hao</creatorcontrib><creatorcontrib>Li, Yuhang</creatorcontrib><creatorcontrib>Li, Chunzhong</creatorcontrib><title>Toward High‐Performance CO2‐to‐C2 Electroreduction via Linker Tuning on MOF‐Derived Catalysts</title><title>Small (Weinheim an der Bergstrasse, Germany)</title><description>Copper (Cu)‐based metal–organic frameworks (MOFs) and MOF‐derived catalysts are well studied for electroreduction of carbon dioxide (CO2); however, the effects of organic linkers for the selectivity of CO2 reduction are still unrevealed. Here, a series of Cu‐based MOF‐derived catalysts is investigated with different organic linkers appended, named X‐Cu‐BDC (BDC = 1,4‐benzenedicarboxylic acid, X = NH2, OH, H, F, and 2F). It is found that the linkers affect the faradaic efficiency (FE) for C2 products with an order of NH2 < OH < bare Cu‐BDC < F < 2F, thus tuning the FEC2:FEC1 ratios from 0.6 to 3.8. As a result, the highest C2 FE of ≈63% at a current density of 150 mA cm−2 on 2F‐Cu‐BDC derived catalyst is achieved. Using operando Raman measurements, it is revealed that the MOF derives to Cu2O during eCO2RR but organic linkers are stable. The fluorine group in organic linker can promote the H2O dissociation to *H species, further facilitating the hydrogenation of *CO to *CHO that helps CC coupling.
The organic linker effects on Cu‐1,4‐benzene dicarboxylate metal–organic frameworks derived catalysts enable electrocatalytic CO2 reduction to multicarbon products including ethylene, ethanol with a total C2 faradaic efficiency of about 63% at a current density of 150 mA cm−2.</description><subject>C 2 products</subject><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>CO 2 electroreduction</subject><subject>Copper</subject><subject>Cu metal–organic frameworks</subject><subject>Electrowinning</subject><subject>Fluorine</subject><subject>Metal-organic frameworks</subject><subject>Nanotechnology</subject><subject>organic linkers</subject><subject>Selectivity</subject><subject>Tuning</subject><issn>1613-6810</issn><issn>1613-6829</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNpdkL9OwzAQhyMEEqWwMkdiYWmxz4mTjChQipSqSJTZcpxLcUniYietuvEIPCNPQqqiDiz356dPp9PnedeUjCkhcOfqqhoDASAkAnLiDSinbMRjSE6PMyXn3oVzK0IYhSAaeLgwW2kLf6qX7z9f3y9oS2Nr2Sj00zn0SWv6koL_WKFqrbFYdKrVpvE3WvqZbj7Q-ouu0c3S78PZfNLjD2j1Bgs_la2sdq51l95ZKSuHV3996L1NHhfpdJTNn57T-2y0Bs7JqGQyiGWeR2HBeQmE5VDSOIhUwGLEkiqCGKMsoGCQBHkEpSpDFStUOcMoSdjQuz3cXVvz2aFrRa2dwqqSDZrOCeABTwLGEujRm3_oynS26b_rqTAJopBx1lPJgdrqCndibXUt7U5QIvbKxV65OCoXr7MsO27sF2bWe58</recordid><startdate>20220501</startdate><enddate>20220501</enddate><creator>Chen, Rongzhen</creator><creator>Cheng, Ling</creator><creator>Liu, Jinze</creator><creator>Wang, Yating</creator><creator>Ge, Wangxin</creator><creator>Xiao, Chuqian</creator><creator>Jiang, Hao</creator><creator>Li, Yuhang</creator><creator>Li, Chunzhong</creator><general>Wiley Subscription Services, Inc</general><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-7897-5850</orcidid></search><sort><creationdate>20220501</creationdate><title>Toward High‐Performance CO2‐to‐C2 Electroreduction via Linker Tuning on MOF‐Derived Catalysts</title><author>Chen, Rongzhen ; Cheng, Ling ; Liu, Jinze ; Wang, Yating ; Ge, Wangxin ; Xiao, Chuqian ; Jiang, Hao ; Li, Yuhang ; Li, Chunzhong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p2660-f3a48abb75d66f203b2f1847c438eef1c0ee8ead2d3294b72fcf5c8cecb3e7993</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>C 2 products</topic><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>CO 2 electroreduction</topic><topic>Copper</topic><topic>Cu metal–organic frameworks</topic><topic>Electrowinning</topic><topic>Fluorine</topic><topic>Metal-organic frameworks</topic><topic>Nanotechnology</topic><topic>organic linkers</topic><topic>Selectivity</topic><topic>Tuning</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chen, Rongzhen</creatorcontrib><creatorcontrib>Cheng, Ling</creatorcontrib><creatorcontrib>Liu, Jinze</creatorcontrib><creatorcontrib>Wang, Yating</creatorcontrib><creatorcontrib>Ge, Wangxin</creatorcontrib><creatorcontrib>Xiao, Chuqian</creatorcontrib><creatorcontrib>Jiang, Hao</creatorcontrib><creatorcontrib>Li, Yuhang</creatorcontrib><creatorcontrib>Li, Chunzhong</creatorcontrib><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>Small (Weinheim an der Bergstrasse, Germany)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chen, Rongzhen</au><au>Cheng, Ling</au><au>Liu, Jinze</au><au>Wang, Yating</au><au>Ge, Wangxin</au><au>Xiao, Chuqian</au><au>Jiang, Hao</au><au>Li, Yuhang</au><au>Li, Chunzhong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Toward High‐Performance CO2‐to‐C2 Electroreduction via Linker Tuning on MOF‐Derived Catalysts</atitle><jtitle>Small (Weinheim an der Bergstrasse, Germany)</jtitle><date>2022-05-01</date><risdate>2022</risdate><volume>18</volume><issue>18</issue><spage>e2200720</spage><epage>n/a</epage><pages>e2200720-n/a</pages><issn>1613-6810</issn><eissn>1613-6829</eissn><abstract>Copper (Cu)‐based metal–organic frameworks (MOFs) and MOF‐derived catalysts are well studied for electroreduction of carbon dioxide (CO2); however, the effects of organic linkers for the selectivity of CO2 reduction are still unrevealed. Here, a series of Cu‐based MOF‐derived catalysts is investigated with different organic linkers appended, named X‐Cu‐BDC (BDC = 1,4‐benzenedicarboxylic acid, X = NH2, OH, H, F, and 2F). It is found that the linkers affect the faradaic efficiency (FE) for C2 products with an order of NH2 < OH < bare Cu‐BDC < F < 2F, thus tuning the FEC2:FEC1 ratios from 0.6 to 3.8. As a result, the highest C2 FE of ≈63% at a current density of 150 mA cm−2 on 2F‐Cu‐BDC derived catalyst is achieved. Using operando Raman measurements, it is revealed that the MOF derives to Cu2O during eCO2RR but organic linkers are stable. The fluorine group in organic linker can promote the H2O dissociation to *H species, further facilitating the hydrogenation of *CO to *CHO that helps CC coupling.
The organic linker effects on Cu‐1,4‐benzene dicarboxylate metal–organic frameworks derived catalysts enable electrocatalytic CO2 reduction to multicarbon products including ethylene, ethanol with a total C2 faradaic efficiency of about 63% at a current density of 150 mA cm−2.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/smll.202200720</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0001-7897-5850</orcidid></addata></record> |
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| subjects | C 2 products Carbon dioxide Catalysts CO 2 electroreduction Copper Cu metal–organic frameworks Electrowinning Fluorine Metal-organic frameworks Nanotechnology organic linkers Selectivity Tuning |
| title | Toward High‐Performance CO2‐to‐C2 Electroreduction via Linker Tuning on MOF‐Derived Catalysts |
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