Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis
A series of stable heterometallic Fe2M cluster‐based MOFs (NNU‐31‐M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and p...
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| Veröffentlicht in: | Angewandte Chemie International Edition 2020-02, Vol.59 (7), p.2659-2663 |
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| creator | Dong, Long‐Zhang Zhang, Lei Liu, Jiang Huang, Qing Lu, Meng Ji, Wen‐Xin Lan, Ya‐Qian |
| description | A series of stable heterometallic Fe2M cluster‐based MOFs (NNU‐31‐M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and photosensitive ligands excited by visible light generate separated electrons and holes. Then, low‐valent metal M accepts electrons to reduce CO2, and high‐valent Fe uses holes to oxidize H2O. This is the first MOF photocatalyst system to finish artificial photosynthetic full reaction. It is noted that NNU‐31‐Zn exhibits the highest HCOOH yield of 26.3 μmol g−1 h−1 (selectivity of ca. 100 %). Furthermore, the DFT calculations based on crystal structures demonstrate the photocatalytic reaction mechanism. This work proposes a new strategy for how to design crystalline photocatalyst to realize artificial photosynthetic overall reaction.
A series of stable heterometallic Fe2M cluster‐based MOFs achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. A strategy is proposed to design crystalline photocatalysts to realize the overall artificial photosynthetic reaction. |
| doi_str_mv | 10.1002/anie.201913284 |
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A series of stable heterometallic Fe2M cluster‐based MOFs achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. A strategy is proposed to design crystalline photocatalysts to realize the overall artificial photosynthetic reaction.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.201913284</identifier><identifier>PMID: 31797510</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Carbon dioxide ; carbon dioxide reduction ; Catalysts ; Clusters ; Crystal structure ; Electrons ; heterometallic catalysts ; Iron ; Metal-organic frameworks ; Photocatalysis ; Photocatalysts ; Photosensitivity ; Photosynthesis ; Reaction mechanisms ; Reagents ; Selectivity ; Zinc</subject><ispartof>Angewandte Chemie International Edition, 2020-02, Vol.59 (7), p.2659-2663</ispartof><rights>2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.</rights><rights>2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c4764-d1efda709b06399faa5c62fd28d2021a0a9dc4161c7d441396890a0bd1f632893</citedby><cites>FETCH-LOGICAL-c4764-d1efda709b06399faa5c62fd28d2021a0a9dc4161c7d441396890a0bd1f632893</cites><orcidid>0000-0002-2140-7980</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.201913284$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.201913284$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27923,27924,45573,45574</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/31797510$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Dong, Long‐Zhang</creatorcontrib><creatorcontrib>Zhang, Lei</creatorcontrib><creatorcontrib>Liu, Jiang</creatorcontrib><creatorcontrib>Huang, Qing</creatorcontrib><creatorcontrib>Lu, Meng</creatorcontrib><creatorcontrib>Ji, Wen‐Xin</creatorcontrib><creatorcontrib>Lan, Ya‐Qian</creatorcontrib><title>Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>A series of stable heterometallic Fe2M cluster‐based MOFs (NNU‐31‐M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and photosensitive ligands excited by visible light generate separated electrons and holes. Then, low‐valent metal M accepts electrons to reduce CO2, and high‐valent Fe uses holes to oxidize H2O. This is the first MOF photocatalyst system to finish artificial photosynthetic full reaction. It is noted that NNU‐31‐Zn exhibits the highest HCOOH yield of 26.3 μmol g−1 h−1 (selectivity of ca. 100 %). Furthermore, the DFT calculations based on crystal structures demonstrate the photocatalytic reaction mechanism. This work proposes a new strategy for how to design crystalline photocatalyst to realize artificial photosynthetic overall reaction.
A series of stable heterometallic Fe2M cluster‐based MOFs achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. A strategy is proposed to design crystalline photocatalysts to realize the overall artificial photosynthetic reaction.</description><subject>Carbon dioxide</subject><subject>carbon dioxide reduction</subject><subject>Catalysts</subject><subject>Clusters</subject><subject>Crystal structure</subject><subject>Electrons</subject><subject>heterometallic catalysts</subject><subject>Iron</subject><subject>Metal-organic frameworks</subject><subject>Photocatalysis</subject><subject>Photocatalysts</subject><subject>Photosensitivity</subject><subject>Photosynthesis</subject><subject>Reaction mechanisms</subject><subject>Reagents</subject><subject>Selectivity</subject><subject>Zinc</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqFkM9OGzEQh62qVUNDrz2ilXrhsumMvbteH0MEBQkBUsvZcmwvOPXG1N5VlBuP0Gfsk2AU_khcOHlkffObmY-QbwgzBKA_1NrZGQUUyGhbfSB7WFMsGefsY64rxkre1jghX1JaZb5toflMJgy54DXCHpG_BrX0tji1g42ht4Py3uli4ceUP_7f_ztSyZriMt7kSbo4iaq3mxD_FAuV0W0aUtGFWMzj4DqnnfLF1W0YQtquh1ubXNonnzrlk_369E7J9cnx78VpeX7582wxPy91xZuqNGg7oziIJTRMiE6pWje0M7Q1FCgqUMLoChvU3FQVMtG0AhQsDXZNPlywKTnc5d7F8He0aZC9S9p6r9Y2jElSRrHhUHPI6Pc36CqMcZ23y1QNUAmRvU3JbEfpGFKKtpN30fUqbiWCfFQvH9XLF_W54eApdlz21rzgz64zIHbAxnm7fSdOzi_Ojl_DHwCaypET</recordid><startdate>20200210</startdate><enddate>20200210</enddate><creator>Dong, Long‐Zhang</creator><creator>Zhang, Lei</creator><creator>Liu, Jiang</creator><creator>Huang, Qing</creator><creator>Lu, Meng</creator><creator>Ji, Wen‐Xin</creator><creator>Lan, Ya‐Qian</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/0000-0002-2140-7980</orcidid></search><sort><creationdate>20200210</creationdate><title>Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis</title><author>Dong, Long‐Zhang ; Zhang, Lei ; Liu, Jiang ; Huang, Qing ; Lu, Meng ; Ji, Wen‐Xin ; Lan, Ya‐Qian</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4764-d1efda709b06399faa5c62fd28d2021a0a9dc4161c7d441396890a0bd1f632893</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Carbon dioxide</topic><topic>carbon dioxide reduction</topic><topic>Catalysts</topic><topic>Clusters</topic><topic>Crystal structure</topic><topic>Electrons</topic><topic>heterometallic catalysts</topic><topic>Iron</topic><topic>Metal-organic frameworks</topic><topic>Photocatalysis</topic><topic>Photocatalysts</topic><topic>Photosensitivity</topic><topic>Photosynthesis</topic><topic>Reaction mechanisms</topic><topic>Reagents</topic><topic>Selectivity</topic><topic>Zinc</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Dong, Long‐Zhang</creatorcontrib><creatorcontrib>Zhang, Lei</creatorcontrib><creatorcontrib>Liu, Jiang</creatorcontrib><creatorcontrib>Huang, Qing</creatorcontrib><creatorcontrib>Lu, Meng</creatorcontrib><creatorcontrib>Ji, Wen‐Xin</creatorcontrib><creatorcontrib>Lan, Ya‐Qian</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>Dong, Long‐Zhang</au><au>Zhang, Lei</au><au>Liu, Jiang</au><au>Huang, Qing</au><au>Lu, Meng</au><au>Ji, Wen‐Xin</au><au>Lan, Ya‐Qian</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2020-02-10</date><risdate>2020</risdate><volume>59</volume><issue>7</issue><spage>2659</spage><epage>2663</epage><pages>2659-2663</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>A series of stable heterometallic Fe2M cluster‐based MOFs (NNU‐31‐M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and photosensitive ligands excited by visible light generate separated electrons and holes. Then, low‐valent metal M accepts electrons to reduce CO2, and high‐valent Fe uses holes to oxidize H2O. This is the first MOF photocatalyst system to finish artificial photosynthetic full reaction. It is noted that NNU‐31‐Zn exhibits the highest HCOOH yield of 26.3 μmol g−1 h−1 (selectivity of ca. 100 %). Furthermore, the DFT calculations based on crystal structures demonstrate the photocatalytic reaction mechanism. This work proposes a new strategy for how to design crystalline photocatalyst to realize artificial photosynthetic overall reaction.
A series of stable heterometallic Fe2M cluster‐based MOFs achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. A strategy is proposed to design crystalline photocatalysts to realize the overall artificial photosynthetic reaction.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>31797510</pmid><doi>10.1002/anie.201913284</doi><tpages>5</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-2140-7980</orcidid></addata></record> |
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| subjects | Carbon dioxide carbon dioxide reduction Catalysts Clusters Crystal structure Electrons heterometallic catalysts Iron Metal-organic frameworks Photocatalysis Photocatalysts Photosensitivity Photosynthesis Reaction mechanisms Reagents Selectivity Zinc |
| title | Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis |
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