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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| Published in | Angewandte Chemie International Edition Vol. 59; no. 7; pp. 2659 - 2663 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Germany
Wiley Subscription Services, Inc
10.02.2020
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| Edition | International ed. in English |
| Subjects | |
| Online Access | Get full text |
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| 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. |
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| AbstractList | 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. A series of stable heterometallic Fe M cluster-based MOFs (NNU-31-M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO and H O into HCOOH and O 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 CO , and high-valent Fe uses holes to oxidize H O. 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 h (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 Fe2 M cluster-based MOFs (NNU-31-M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2 O 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 H2 O. 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 Fe2 M cluster-based MOFs (NNU-31-M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2 O 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 H2 O. 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 (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 Fe 2 M cluster‐based MOFs ( NNU‐31‐M , M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO 2 and H 2 O into HCOOH and O 2 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 CO 2 , and high‐valent Fe uses holes to oxidize H 2 O. 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. |
| Author | Huang, Qing Lu, Meng Lan, Ya‐Qian Liu, Jiang Ji, Wen‐Xin Dong, Long‐Zhang Zhang, Lei |
| Author_xml | – sequence: 1 givenname: Long‐Zhang surname: Dong fullname: Dong, Long‐Zhang organization: Nanjing Normal University – sequence: 2 givenname: Lei surname: Zhang fullname: Zhang, Lei organization: Nanjing Normal University – sequence: 3 givenname: Jiang surname: Liu fullname: Liu, Jiang email: liuj@njnu.edu.cn organization: Nanjing Normal University – sequence: 4 givenname: Qing surname: Huang fullname: Huang, Qing organization: Nanjing Normal University – sequence: 5 givenname: Meng surname: Lu fullname: Lu, Meng organization: Nanjing Normal University – sequence: 6 givenname: Wen‐Xin surname: Ji fullname: Ji, Wen‐Xin organization: Ningxia University – sequence: 7 givenname: Ya‐Qian orcidid: 0000-0002-2140-7980 surname: Lan fullname: Lan, Ya‐Qian email: yqlan@njnu.edu.cn organization: Nanjing Normal University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31797510$$D View this record in MEDLINE/PubMed |
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| Copyright | 2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. 2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim |
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| Keywords | heterometallic catalysts carbon dioxide reduction photocatalysts metal-organic frameworks |
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| Snippet | 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... A series of stable heterometallic Fe 2 M cluster‐based MOFs ( NNU‐31‐M , M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of... A series of stable heterometallic Fe M cluster-based MOFs (NNU-31-M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO... A series of stable heterometallic Fe2 M cluster-based MOFs (NNU-31-M, M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of... |
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| SubjectTerms | Carbon dioxide carbon dioxide reduction Catalysts Clusters Crystal structure Electrons heterometallic catalysts Iron Metal-organic frameworks Photocatalysis Photocatalysts Photosensitivity Photosynthesis Reaction mechanisms Reagents Selectivity |
| Title | Stable Heterometallic Cluster‐Based Organic Framework Catalysts for Artificial Photosynthesis |
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