Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability
We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co–N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90%...
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| Veröffentlicht in: | Journal of the American Chemical Society 2018-03, Vol.140 (12), p.4218-4221 |
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| creator | Pan, Yuan Lin, Rui Chen, Yinjuan Liu, Shoujie Zhu, Wei Cao, Xing Chen, Wenxing Wu, Konglin Cheong, Weng-Chon Wang, Yu Zheng, Lirong Luo, Jun Lin, Yan Liu, Yunqi Liu, Chenguang Li, Jun Lu, Qi Chen, Xin Wang, Dingsheng Peng, Qing Chen, Chen Li, Yadong |
| description | We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co–N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from −0.57 to −0.88 V (the FECO exceeded 99% at −0.73 and −0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co–N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH* as well as the desorption of CO. |
| doi_str_mv | 10.1021/jacs.8b00814 |
| format | Article |
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Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from −0.57 to −0.88 V (the FECO exceeded 99% at −0.73 and −0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co–N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH* as well as the desorption of CO.</description><identifier>ISSN: 0002-7863</identifier><identifier>EISSN: 1520-5126</identifier><identifier>DOI: 10.1021/jacs.8b00814</identifier><language>eng</language><publisher>American Chemical Society</publisher><ispartof>Journal of the American Chemical Society, 2018-03, Vol.140 (12), p.4218-4221</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0003-1544-1127 ; 0000-0002-8456-3980 ; 0000-0003-0074-7633</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/jacs.8b00814$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/jacs.8b00814$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>315,781,785,27081,27929,27930,56743,56793</link.rule.ids></links><search><creatorcontrib>Pan, Yuan</creatorcontrib><creatorcontrib>Lin, Rui</creatorcontrib><creatorcontrib>Chen, Yinjuan</creatorcontrib><creatorcontrib>Liu, Shoujie</creatorcontrib><creatorcontrib>Zhu, Wei</creatorcontrib><creatorcontrib>Cao, Xing</creatorcontrib><creatorcontrib>Chen, Wenxing</creatorcontrib><creatorcontrib>Wu, Konglin</creatorcontrib><creatorcontrib>Cheong, Weng-Chon</creatorcontrib><creatorcontrib>Wang, Yu</creatorcontrib><creatorcontrib>Zheng, Lirong</creatorcontrib><creatorcontrib>Luo, Jun</creatorcontrib><creatorcontrib>Lin, Yan</creatorcontrib><creatorcontrib>Liu, Yunqi</creatorcontrib><creatorcontrib>Liu, Chenguang</creatorcontrib><creatorcontrib>Li, Jun</creatorcontrib><creatorcontrib>Lu, Qi</creatorcontrib><creatorcontrib>Chen, Xin</creatorcontrib><creatorcontrib>Wang, Dingsheng</creatorcontrib><creatorcontrib>Peng, Qing</creatorcontrib><creatorcontrib>Chen, Chen</creatorcontrib><creatorcontrib>Li, Yadong</creatorcontrib><title>Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability</title><title>Journal of the American Chemical Society</title><addtitle>J. Am. Chem. Soc</addtitle><description>We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co–N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from −0.57 to −0.88 V (the FECO exceeded 99% at −0.73 and −0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co–N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH* as well as the desorption of CO.</description><issn>0002-7863</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNpFkE1OwzAQRi0EEqWw4wDeILEJ2JPGTthV4VeqqNTCOrIdu7i4McQOqDuugLghJyGFSqxGn943o9FD6JiSM0qAni-FCme5JCSnox00oBmQJKPAdtGAEAIJz1m6jw5CWPZxBDkdoM9LHeyiwd7guW0WTifj6Fe49N8fX_cZLkUUbh2t6mnUF3iMZ152IeIrp1VsvfrlfTa-xeUU8EzXnYrWN_jdxid8r0Xr1pgSctJjPNebNftm4xqLpu7bK9E-C-k0nkchrevBIdozwgV9tJ1D9Hh99VDeJpPpzV05niSC8jQmqeIjoEwVilPDagacFGBYYbRUzKSp4bI2GQOTFZAVkhlVi5wzJjOjBDCSDtHp392X1r92OsRqZYPSzolG-y5UQCgUlHCA_2rvt1r6rm36xypKqo31amO92lpPfwD8MXZR</recordid><startdate>20180328</startdate><enddate>20180328</enddate><creator>Pan, Yuan</creator><creator>Lin, Rui</creator><creator>Chen, Yinjuan</creator><creator>Liu, Shoujie</creator><creator>Zhu, Wei</creator><creator>Cao, Xing</creator><creator>Chen, Wenxing</creator><creator>Wu, Konglin</creator><creator>Cheong, Weng-Chon</creator><creator>Wang, Yu</creator><creator>Zheng, Lirong</creator><creator>Luo, Jun</creator><creator>Lin, Yan</creator><creator>Liu, Yunqi</creator><creator>Liu, Chenguang</creator><creator>Li, Jun</creator><creator>Lu, Qi</creator><creator>Chen, Xin</creator><creator>Wang, Dingsheng</creator><creator>Peng, Qing</creator><creator>Chen, Chen</creator><creator>Li, Yadong</creator><general>American Chemical Society</general><scope>7X8</scope><orcidid>https://orcid.org/0000-0003-1544-1127</orcidid><orcidid>https://orcid.org/0000-0002-8456-3980</orcidid><orcidid>https://orcid.org/0000-0003-0074-7633</orcidid></search><sort><creationdate>20180328</creationdate><title>Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability</title><author>Pan, Yuan ; Lin, Rui ; Chen, Yinjuan ; Liu, Shoujie ; Zhu, Wei ; Cao, Xing ; Chen, Wenxing ; Wu, Konglin ; Cheong, Weng-Chon ; Wang, Yu ; Zheng, Lirong ; Luo, Jun ; Lin, Yan ; Liu, Yunqi ; Liu, Chenguang ; Li, Jun ; Lu, Qi ; Chen, Xin ; Wang, Dingsheng ; Peng, Qing ; Chen, Chen ; Li, Yadong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a173t-3c74216c9c71f6d627092f69febc6f33f7bdf562f59259b6fcda8766b5fca2603</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Pan, Yuan</creatorcontrib><creatorcontrib>Lin, Rui</creatorcontrib><creatorcontrib>Chen, Yinjuan</creatorcontrib><creatorcontrib>Liu, Shoujie</creatorcontrib><creatorcontrib>Zhu, Wei</creatorcontrib><creatorcontrib>Cao, Xing</creatorcontrib><creatorcontrib>Chen, Wenxing</creatorcontrib><creatorcontrib>Wu, Konglin</creatorcontrib><creatorcontrib>Cheong, Weng-Chon</creatorcontrib><creatorcontrib>Wang, Yu</creatorcontrib><creatorcontrib>Zheng, Lirong</creatorcontrib><creatorcontrib>Luo, Jun</creatorcontrib><creatorcontrib>Lin, Yan</creatorcontrib><creatorcontrib>Liu, Yunqi</creatorcontrib><creatorcontrib>Liu, Chenguang</creatorcontrib><creatorcontrib>Li, Jun</creatorcontrib><creatorcontrib>Lu, Qi</creatorcontrib><creatorcontrib>Chen, Xin</creatorcontrib><creatorcontrib>Wang, Dingsheng</creatorcontrib><creatorcontrib>Peng, Qing</creatorcontrib><creatorcontrib>Chen, Chen</creatorcontrib><creatorcontrib>Li, Yadong</creatorcontrib><collection>MEDLINE - Academic</collection><jtitle>Journal of the American Chemical Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Pan, Yuan</au><au>Lin, Rui</au><au>Chen, Yinjuan</au><au>Liu, Shoujie</au><au>Zhu, Wei</au><au>Cao, Xing</au><au>Chen, Wenxing</au><au>Wu, Konglin</au><au>Cheong, Weng-Chon</au><au>Wang, Yu</au><au>Zheng, Lirong</au><au>Luo, Jun</au><au>Lin, Yan</au><au>Liu, Yunqi</au><au>Liu, Chenguang</au><au>Li, Jun</au><au>Lu, Qi</au><au>Chen, Xin</au><au>Wang, Dingsheng</au><au>Peng, Qing</au><au>Chen, Chen</au><au>Li, Yadong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J. Am. Chem. Soc</addtitle><date>2018-03-28</date><risdate>2018</risdate><volume>140</volume><issue>12</issue><spage>4218</spage><epage>4221</epage><pages>4218-4221</pages><issn>0002-7863</issn><eissn>1520-5126</eissn><abstract>We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co–N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from −0.57 to −0.88 V (the FECO exceeded 99% at −0.73 and −0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co–N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH* as well as the desorption of CO.</abstract><pub>American Chemical Society</pub><doi>10.1021/jacs.8b00814</doi><tpages>4</tpages><orcidid>https://orcid.org/0000-0003-1544-1127</orcidid><orcidid>https://orcid.org/0000-0002-8456-3980</orcidid><orcidid>https://orcid.org/0000-0003-0074-7633</orcidid></addata></record> |
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| title | Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability |
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