Heterogenization of Salen Metal Molecular Catalysts in Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution
Integrating a molecular catalyst with a light harvester into a photocatalyst is an effective strategy for solar light conversion. However, it is challenging to establish a crystallized framework with well‐organized connections that favour charge separation and transfer. Herein, we report the heterog...
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| Veröffentlicht in: | Angewandte Chemie International Edition 2023-01, Vol.62 (3), p.e202214143-n/a |
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| creator | Zhou, Wei Deng, Qi‐Wen He, Hui‐Jie Yang, Li Liu, Tian‐Yi Wang, Xiao Zheng, Dao‐Yuan Dai, Zhang‐Ben Sun, Lei Liu, Chengcheng Wu, Hao Li, Zhen Deng, Wei‐Qiao |
| description | Integrating a molecular catalyst with a light harvester into a photocatalyst is an effective strategy for solar light conversion. However, it is challenging to establish a crystallized framework with well‐organized connections that favour charge separation and transfer. Herein, we report the heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution. The chemically conjugated bonds between the two units contribute to fast photogenerated electron transfer and thereby promote the proton reduction reaction. The Salen cobalt‐based COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported nonnoble metal based COF photocatalysts. This work provides a strategy to construct atom‐efficient photocatalysts by the heterogenization of molecular catalysts into covalent organic frameworks.
The heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution is reported. Co/Zn‐Salen‐COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported non‐noble metal‐based COF photocatalysts |
| doi_str_mv | 10.1002/anie.202214143 |
| format | Article |
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The heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution is reported. Co/Zn‐Salen‐COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported non‐noble metal‐based COF photocatalysts</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202214143</identifier><identifier>PMID: 36401588</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Catalysts ; Charge transfer ; Chemical bonds ; Chemical reduction ; Cobalt ; Covalence ; Covalent Organic Frameworks ; Crystallization ; Electron transfer ; Energy harvesting ; Evolution ; Harvesters ; Heterogenization ; Hydrogen ; Hydrogen evolution ; Molecular Catalyst ; Photocatalysis ; Photocatalysts ; Photocatalytic Hydrogen Evolution</subject><ispartof>Angewandte Chemie International Edition, 2023-01, Vol.62 (3), p.e202214143-n/a</ispartof><rights>2022 Wiley‐VCH GmbH</rights><rights>2022 Wiley-VCH GmbH.</rights><rights>2023 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3733-c2b70641b38baf68769e2063f3e4a53e545353187f677e341d22174b817e3bb3</citedby><cites>FETCH-LOGICAL-c3733-c2b70641b38baf68769e2063f3e4a53e545353187f677e341d22174b817e3bb3</cites><orcidid>0000-0002-3671-5951</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%2Fanie.202214143$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202214143$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>315,781,785,1418,27929,27930,45579,45580</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36401588$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhou, Wei</creatorcontrib><creatorcontrib>Deng, Qi‐Wen</creatorcontrib><creatorcontrib>He, Hui‐Jie</creatorcontrib><creatorcontrib>Yang, Li</creatorcontrib><creatorcontrib>Liu, Tian‐Yi</creatorcontrib><creatorcontrib>Wang, Xiao</creatorcontrib><creatorcontrib>Zheng, Dao‐Yuan</creatorcontrib><creatorcontrib>Dai, Zhang‐Ben</creatorcontrib><creatorcontrib>Sun, Lei</creatorcontrib><creatorcontrib>Liu, Chengcheng</creatorcontrib><creatorcontrib>Wu, Hao</creatorcontrib><creatorcontrib>Li, Zhen</creatorcontrib><creatorcontrib>Deng, Wei‐Qiao</creatorcontrib><title>Heterogenization of Salen Metal Molecular Catalysts in Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>Integrating a molecular catalyst with a light harvester into a photocatalyst is an effective strategy for solar light conversion. However, it is challenging to establish a crystallized framework with well‐organized connections that favour charge separation and transfer. Herein, we report the heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution. The chemically conjugated bonds between the two units contribute to fast photogenerated electron transfer and thereby promote the proton reduction reaction. The Salen cobalt‐based COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported nonnoble metal based COF photocatalysts. This work provides a strategy to construct atom‐efficient photocatalysts by the heterogenization of molecular catalysts into covalent organic frameworks.
The heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution is reported. Co/Zn‐Salen‐COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported non‐noble metal‐based COF photocatalysts</description><subject>Catalysts</subject><subject>Charge transfer</subject><subject>Chemical bonds</subject><subject>Chemical reduction</subject><subject>Cobalt</subject><subject>Covalence</subject><subject>Covalent Organic Frameworks</subject><subject>Crystallization</subject><subject>Electron transfer</subject><subject>Energy harvesting</subject><subject>Evolution</subject><subject>Harvesters</subject><subject>Heterogenization</subject><subject>Hydrogen</subject><subject>Hydrogen evolution</subject><subject>Molecular Catalyst</subject><subject>Photocatalysis</subject><subject>Photocatalysts</subject><subject>Photocatalytic Hydrogen Evolution</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNqFkb1PwzAQxS0E4qOwMiJLLCwt_krsjKgqFIlSJLpHTnopKW4MdtJS_nocWorEwnR38u_ePfkhdE5JjxLCrnVVQo8Rxqiggu-hYxox2uVS8v3QC867UkX0CJ14Pw-8UiQ-REc8FoRGSh2jjyHU4OwMqvJT16WtsC3wszZQ4RHU2uCRNZA3Rjvc12Fe-9rjssJ9u2yhGo_dLHjI8a3TC1hZ9-pxYR1-erG1zb836vA6XE-_j-DB0pqmvXOKDgptPJxtawdNbgeT_rD7ML677988dHMug_ucZZLEgmZcZbqIlYwTYCTmBQehIw6RiHjEqZJFLCVwQafhK6TIFA1TlvEOutrIvjn73oCv00XpczBGV2AbnzLJFU2YYCqgl3_QuW1cFcwFKqaJUipKAtXbULmz3jso0jdXLrRbp5SkbSRpG0m6iyQsXGxlm2wB0x3-k0EAkg2wKg2s_5FLbx7vB7_iX-eSmFQ</recordid><startdate>20230116</startdate><enddate>20230116</enddate><creator>Zhou, Wei</creator><creator>Deng, Qi‐Wen</creator><creator>He, Hui‐Jie</creator><creator>Yang, Li</creator><creator>Liu, Tian‐Yi</creator><creator>Wang, Xiao</creator><creator>Zheng, Dao‐Yuan</creator><creator>Dai, Zhang‐Ben</creator><creator>Sun, Lei</creator><creator>Liu, Chengcheng</creator><creator>Wu, Hao</creator><creator>Li, Zhen</creator><creator>Deng, Wei‐Qiao</creator><general>Wiley Subscription Services, Inc</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-3671-5951</orcidid></search><sort><creationdate>20230116</creationdate><title>Heterogenization of Salen Metal Molecular Catalysts in Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution</title><author>Zhou, Wei ; Deng, Qi‐Wen ; He, Hui‐Jie ; Yang, Li ; Liu, Tian‐Yi ; Wang, Xiao ; Zheng, Dao‐Yuan ; Dai, Zhang‐Ben ; Sun, Lei ; Liu, Chengcheng ; Wu, Hao ; Li, Zhen ; Deng, Wei‐Qiao</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3733-c2b70641b38baf68769e2063f3e4a53e545353187f677e341d22174b817e3bb3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Catalysts</topic><topic>Charge transfer</topic><topic>Chemical bonds</topic><topic>Chemical reduction</topic><topic>Cobalt</topic><topic>Covalence</topic><topic>Covalent Organic Frameworks</topic><topic>Crystallization</topic><topic>Electron transfer</topic><topic>Energy harvesting</topic><topic>Evolution</topic><topic>Harvesters</topic><topic>Heterogenization</topic><topic>Hydrogen</topic><topic>Hydrogen evolution</topic><topic>Molecular Catalyst</topic><topic>Photocatalysis</topic><topic>Photocatalysts</topic><topic>Photocatalytic Hydrogen Evolution</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhou, Wei</creatorcontrib><creatorcontrib>Deng, Qi‐Wen</creatorcontrib><creatorcontrib>He, Hui‐Jie</creatorcontrib><creatorcontrib>Yang, Li</creatorcontrib><creatorcontrib>Liu, Tian‐Yi</creatorcontrib><creatorcontrib>Wang, Xiao</creatorcontrib><creatorcontrib>Zheng, Dao‐Yuan</creatorcontrib><creatorcontrib>Dai, Zhang‐Ben</creatorcontrib><creatorcontrib>Sun, Lei</creatorcontrib><creatorcontrib>Liu, Chengcheng</creatorcontrib><creatorcontrib>Wu, Hao</creatorcontrib><creatorcontrib>Li, Zhen</creatorcontrib><creatorcontrib>Deng, Wei‐Qiao</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhou, Wei</au><au>Deng, Qi‐Wen</au><au>He, Hui‐Jie</au><au>Yang, Li</au><au>Liu, Tian‐Yi</au><au>Wang, Xiao</au><au>Zheng, Dao‐Yuan</au><au>Dai, Zhang‐Ben</au><au>Sun, Lei</au><au>Liu, Chengcheng</au><au>Wu, Hao</au><au>Li, Zhen</au><au>Deng, Wei‐Qiao</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Heterogenization of Salen Metal Molecular Catalysts in Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2023-01-16</date><risdate>2023</risdate><volume>62</volume><issue>3</issue><spage>e202214143</spage><epage>n/a</epage><pages>e202214143-n/a</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Integrating a molecular catalyst with a light harvester into a photocatalyst is an effective strategy for solar light conversion. However, it is challenging to establish a crystallized framework with well‐organized connections that favour charge separation and transfer. Herein, we report the heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution. The chemically conjugated bonds between the two units contribute to fast photogenerated electron transfer and thereby promote the proton reduction reaction. The Salen cobalt‐based COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported nonnoble metal based COF photocatalysts. This work provides a strategy to construct atom‐efficient photocatalysts by the heterogenization of molecular catalysts into covalent organic frameworks.
The heterogenization of a Salen metal complex molecular catalyst into a rigid covalent organic framework (COF) through covalent linkage with the light‐harvesting unit of pyrene for photocatalytic hydrogen evolution is reported. Co/Zn‐Salen‐COF showed the best hydrogen evolution activity (1378 μmol g−1 h−1), which is superior to the previously reported non‐noble metal‐based COF photocatalysts</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>36401588</pmid><doi>10.1002/anie.202214143</doi><tpages>8</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-3671-5951</orcidid></addata></record> |
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| subjects | Catalysts Charge transfer Chemical bonds Chemical reduction Cobalt Covalence Covalent Organic Frameworks Crystallization Electron transfer Energy harvesting Evolution Harvesters Heterogenization Hydrogen Hydrogen evolution Molecular Catalyst Photocatalysis Photocatalysts Photocatalytic Hydrogen Evolution |
| title | Heterogenization of Salen Metal Molecular Catalysts in Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution |
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