Amide-bridged conjugated organic polymers: efficient metal-free catalysts for visible-light-driven CO2 reduction with H2O to CO
The visible-light-driven photoreduction of CO2 to value-added chemicals over metal-free photocatalysts without sacrificial reagents is very interesting, but challenging. Herein, we present amide-bridged conjugated organic polymers (amide-COPs) prepared via self-condensation of amino nitriles in comb...
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| Veröffentlicht in: | Chemical science (Cambridge) 2021-09, Vol.12 (34), p.11548-11553 |
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| creator | Fan, Wen Zhang, Fengtao Wang, Zhen Yu, Xiaoxiao Ji, Guipeng Li, Dongyang Tong, Shengrui Wang, Yingbin Han, Buxing Liu, Zhimin |
| description | The visible-light-driven photoreduction of CO2 to value-added chemicals over metal-free photocatalysts without sacrificial reagents is very interesting, but challenging. Herein, we present amide-bridged conjugated organic polymers (amide-COPs) prepared via self-condensation of amino nitriles in combination with hydrolysis, for the photoreduction of CO2 with H2O without any photosensitizers or sacrificial reagents under visible light irradiation. These catalysts can afford CO as the sole carbonaceous product without H2 generation. Especially, amide-DAMN derived from diaminomaleonitrile exhibited the highest activity for the photoreduction of CO2 to CO with a generation rate of 20.6 μmol g−1 h−1. Experiments and DFT calculations confirmed cyano/amide groups as active sites for CO2 reduction and second amine groups for H2O oxidation, and suggested that superior selectivity towards CO may be attributed to the adjacent redox sites. This work presents a new insight into designing photocatalysts for artificial photosynthesis. |
| doi_str_mv | 10.1039/d1sc02499j |
| format | Article |
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Herein, we present amide-bridged conjugated organic polymers (amide-COPs) prepared via self-condensation of amino nitriles in combination with hydrolysis, for the photoreduction of CO2 with H2O without any photosensitizers or sacrificial reagents under visible light irradiation. These catalysts can afford CO as the sole carbonaceous product without H2 generation. Especially, amide-DAMN derived from diaminomaleonitrile exhibited the highest activity for the photoreduction of CO2 to CO with a generation rate of 20.6 μmol g−1 h−1. Experiments and DFT calculations confirmed cyano/amide groups as active sites for CO2 reduction and second amine groups for H2O oxidation, and suggested that superior selectivity towards CO may be attributed to the adjacent redox sites. This work presents a new insight into designing photocatalysts for artificial photosynthesis.</description><identifier>ISSN: 2041-6520</identifier><identifier>EISSN: 2041-6539</identifier><identifier>DOI: 10.1039/d1sc02499j</identifier><identifier>PMID: 34667557</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Carbon dioxide ; Catalysts ; Chemistry ; Condensates ; Hydrogen production ; Light irradiation ; Nitriles ; Oxidation ; Photocatalysis ; Photocatalysts ; Photosynthesis ; Polymers ; Reagents ; Selectivity</subject><ispartof>Chemical science (Cambridge), 2021-09, Vol.12 (34), p.11548-11553</ispartof><rights>Copyright Royal Society of Chemistry 2021</rights><rights>This journal is © The Royal Society of Chemistry 2021 The Royal Society of Chemistry</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC8447930/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC8447930/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,727,780,784,864,885,27924,27925,53791,53793</link.rule.ids></links><search><creatorcontrib>Fan, Wen</creatorcontrib><creatorcontrib>Zhang, Fengtao</creatorcontrib><creatorcontrib>Wang, Zhen</creatorcontrib><creatorcontrib>Yu, Xiaoxiao</creatorcontrib><creatorcontrib>Ji, Guipeng</creatorcontrib><creatorcontrib>Li, Dongyang</creatorcontrib><creatorcontrib>Tong, Shengrui</creatorcontrib><creatorcontrib>Wang, Yingbin</creatorcontrib><creatorcontrib>Han, Buxing</creatorcontrib><creatorcontrib>Liu, Zhimin</creatorcontrib><title>Amide-bridged conjugated organic polymers: efficient metal-free catalysts for visible-light-driven CO2 reduction with H2O to CO</title><title>Chemical science (Cambridge)</title><description>The visible-light-driven photoreduction of CO2 to value-added chemicals over metal-free photocatalysts without sacrificial reagents is very interesting, but challenging. Herein, we present amide-bridged conjugated organic polymers (amide-COPs) prepared via self-condensation of amino nitriles in combination with hydrolysis, for the photoreduction of CO2 with H2O without any photosensitizers or sacrificial reagents under visible light irradiation. These catalysts can afford CO as the sole carbonaceous product without H2 generation. Especially, amide-DAMN derived from diaminomaleonitrile exhibited the highest activity for the photoreduction of CO2 to CO with a generation rate of 20.6 μmol g−1 h−1. Experiments and DFT calculations confirmed cyano/amide groups as active sites for CO2 reduction and second amine groups for H2O oxidation, and suggested that superior selectivity towards CO may be attributed to the adjacent redox sites. This work presents a new insight into designing photocatalysts for artificial photosynthesis.</description><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>Condensates</subject><subject>Hydrogen production</subject><subject>Light irradiation</subject><subject>Nitriles</subject><subject>Oxidation</subject><subject>Photocatalysis</subject><subject>Photocatalysts</subject><subject>Photosynthesis</subject><subject>Polymers</subject><subject>Reagents</subject><subject>Selectivity</subject><issn>2041-6520</issn><issn>2041-6539</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNpdj01r3DAURUVJaUKaTX-BoJts3OhbVhaBMCRNITCbdm1k6dmjwbYmkjxhVv3rFTQUmrd5B-7lwEXoCyXfKOHmxtPsCBPG7D-gC0YEbZTk5uwfM3KOrnLek3qcU8n0J3TOhVJaSn2Bft_PwUPTp-BH8NjFZb-OtlSMabRLcPgQp9MMKd9iGIbgAiwFz1Ds1AwJADtb8ZRLxkNM-Bhy6CdopjDuSuNTOMKCN1uGE_jVlRAX_BrKDj-xLS6xJp_Rx8FOGa7e_iX69fjwc_PUPG-__9jcPzcHxnVpnNNKeeitVIIRRrjgjLLeS-M5HQaihSO0F9prapwylCrnW9LqVrMepLf8Et399R7Wfgbv6opkp-6QwmzTqYs2dP8nS9h1Yzx2rRDacFIF12-CFF9WyKWbQ3YwTXaBuOaOyVYQyiSltfr1XXUf17TUebWltFFCacb_AA2LiBg</recordid><startdate>20210914</startdate><enddate>20210914</enddate><creator>Fan, Wen</creator><creator>Zhang, Fengtao</creator><creator>Wang, Zhen</creator><creator>Yu, Xiaoxiao</creator><creator>Ji, Guipeng</creator><creator>Li, Dongyang</creator><creator>Tong, Shengrui</creator><creator>Wang, Yingbin</creator><creator>Han, Buxing</creator><creator>Liu, Zhimin</creator><general>Royal Society of Chemistry</general><general>The Royal Society of Chemistry</general><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>7X8</scope><scope>5PM</scope></search><sort><creationdate>20210914</creationdate><title>Amide-bridged conjugated organic polymers: efficient metal-free catalysts for visible-light-driven CO2 reduction with H2O to CO</title><author>Fan, Wen ; Zhang, Fengtao ; Wang, Zhen ; Yu, Xiaoxiao ; Ji, Guipeng ; Li, Dongyang ; Tong, Shengrui ; Wang, Yingbin ; Han, Buxing ; Liu, Zhimin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p237t-cc766deba5642020343212bd59d31ff074c01b47d719c69116cd8087872be5da3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>Chemistry</topic><topic>Condensates</topic><topic>Hydrogen production</topic><topic>Light irradiation</topic><topic>Nitriles</topic><topic>Oxidation</topic><topic>Photocatalysis</topic><topic>Photocatalysts</topic><topic>Photosynthesis</topic><topic>Polymers</topic><topic>Reagents</topic><topic>Selectivity</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Fan, Wen</creatorcontrib><creatorcontrib>Zhang, Fengtao</creatorcontrib><creatorcontrib>Wang, Zhen</creatorcontrib><creatorcontrib>Yu, Xiaoxiao</creatorcontrib><creatorcontrib>Ji, Guipeng</creatorcontrib><creatorcontrib>Li, Dongyang</creatorcontrib><creatorcontrib>Tong, Shengrui</creatorcontrib><creatorcontrib>Wang, Yingbin</creatorcontrib><creatorcontrib>Han, Buxing</creatorcontrib><creatorcontrib>Liu, Zhimin</creatorcontrib><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Chemical science (Cambridge)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Fan, Wen</au><au>Zhang, Fengtao</au><au>Wang, Zhen</au><au>Yu, Xiaoxiao</au><au>Ji, Guipeng</au><au>Li, Dongyang</au><au>Tong, Shengrui</au><au>Wang, Yingbin</au><au>Han, Buxing</au><au>Liu, Zhimin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Amide-bridged conjugated organic polymers: efficient metal-free catalysts for visible-light-driven CO2 reduction with H2O to CO</atitle><jtitle>Chemical science (Cambridge)</jtitle><date>2021-09-14</date><risdate>2021</risdate><volume>12</volume><issue>34</issue><spage>11548</spage><epage>11553</epage><pages>11548-11553</pages><issn>2041-6520</issn><eissn>2041-6539</eissn><abstract>The visible-light-driven photoreduction of CO2 to value-added chemicals over metal-free photocatalysts without sacrificial reagents is very interesting, but challenging. Herein, we present amide-bridged conjugated organic polymers (amide-COPs) prepared via self-condensation of amino nitriles in combination with hydrolysis, for the photoreduction of CO2 with H2O without any photosensitizers or sacrificial reagents under visible light irradiation. These catalysts can afford CO as the sole carbonaceous product without H2 generation. Especially, amide-DAMN derived from diaminomaleonitrile exhibited the highest activity for the photoreduction of CO2 to CO with a generation rate of 20.6 μmol g−1 h−1. Experiments and DFT calculations confirmed cyano/amide groups as active sites for CO2 reduction and second amine groups for H2O oxidation, and suggested that superior selectivity towards CO may be attributed to the adjacent redox sites. This work presents a new insight into designing photocatalysts for artificial photosynthesis.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><pmid>34667557</pmid><doi>10.1039/d1sc02499j</doi><tpages>6</tpages><oa>free_for_read</oa></addata></record> |
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| source | DOAJ Directory of Open Access Journals; PubMed Central Open Access; EZB-FREE-00999 freely available EZB journals; PubMed Central |
| subjects | Carbon dioxide Catalysts Chemistry Condensates Hydrogen production Light irradiation Nitriles Oxidation Photocatalysis Photocatalysts Photosynthesis Polymers Reagents Selectivity |
| title | Amide-bridged conjugated organic polymers: efficient metal-free catalysts for visible-light-driven CO2 reduction with H2O to CO |
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