Solar‐Driven Nitrogen Fixation Catalyzed by Stable Radical‐Containing MOFs: Improved Efficiency Induced by a Structural Transformation
Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a single‐crystal‐to‐single‐crystal transformation to generate Gd‐IHEP‐8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical‐radic...
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| Published in | Angewandte Chemie International Edition Vol. 59; no. 46; pp. 20666 - 20671 |
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| Main Authors | , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Weinheim
Wiley Subscription Services, Inc
09.11.2020
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| Edition | International ed. in English |
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| Abstract | Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a single‐crystal‐to‐single‐crystal transformation to generate Gd‐IHEP‐8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical‐radical interactions, and their long‐lifetime radicals result in wide spectral absorption in the range 200–2500 nm. Gd‐IHEP‐7 and Gd‐IHEP‐8 show excellent activity toward solar‐driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h−1 g−1, respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd‐IHEP‐8 versus Gd‐IHEP‐7 is attributed to intermediates stabilized by enhanced hydrogen bonding.
A single‐crystal‐to‐single‐crystal (SCSC) transformation of stable radical‐containing MOF Gd‐IHEP‐7 generates Gd‐IHEP‐8. It is accompanied by a marked increase in efficiency of sacrificial agent‐free photocatalytic nitrogen fixation to yield NH3 from H2O and N2 under simulated solar light irradiation at ambient temperature. The NH3 production rate of 220 μmol h−1 g−1 for Gd‐IHEP‐8 is a new record for MOF photocatalysts. |
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| AbstractList | Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a single‐crystal‐to‐single‐crystal transformation to generate Gd‐IHEP‐8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical‐radical interactions, and their long‐lifetime radicals result in wide spectral absorption in the range 200–2500 nm. Gd‐IHEP‐7 and Gd‐IHEP‐8 show excellent activity toward solar‐driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h−1 g−1, respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd‐IHEP‐8 versus Gd‐IHEP‐7 is attributed to intermediates stabilized by enhanced hydrogen bonding. Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a single‐crystal‐to‐single‐crystal transformation to generate Gd‐IHEP‐8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical‐radical interactions, and their long‐lifetime radicals result in wide spectral absorption in the range 200–2500 nm. Gd‐IHEP‐7 and Gd‐IHEP‐8 show excellent activity toward solar‐driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h−1 g−1, respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd‐IHEP‐8 versus Gd‐IHEP‐7 is attributed to intermediates stabilized by enhanced hydrogen bonding. A single‐crystal‐to‐single‐crystal (SCSC) transformation of stable radical‐containing MOF Gd‐IHEP‐7 generates Gd‐IHEP‐8. It is accompanied by a marked increase in efficiency of sacrificial agent‐free photocatalytic nitrogen fixation to yield NH3 from H2O and N2 under simulated solar light irradiation at ambient temperature. The NH3 production rate of 220 μmol h−1 g−1 for Gd‐IHEP‐8 is a new record for MOF photocatalysts. Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a single‐crystal‐to‐single‐crystal transformation to generate Gd‐IHEP‐8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical‐radical interactions, and their long‐lifetime radicals result in wide spectral absorption in the range 200–2500 nm. Gd‐IHEP‐7 and Gd‐IHEP‐8 show excellent activity toward solar‐driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h −1 g −1 , respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd‐IHEP‐8 versus Gd‐IHEP‐7 is attributed to intermediates stabilized by enhanced hydrogen bonding. Herein we present a new viologen-based radical-containing metal-organic framework (RMOF) Gd-IHEP-7, which upon heating in air undergoes a single-crystal-to-single-crystal transformation to generate Gd-IHEP-8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical-radical interactions, and their long-lifetime radicals result in wide spectral absorption in the range 200-2500 nm. Gd-IHEP-7 and Gd-IHEP-8 show excellent activity toward solar-driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h-1 g-1 , respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd-IHEP-8 versus Gd-IHEP-7 is attributed to intermediates stabilized by enhanced hydrogen bonding.Herein we present a new viologen-based radical-containing metal-organic framework (RMOF) Gd-IHEP-7, which upon heating in air undergoes a single-crystal-to-single-crystal transformation to generate Gd-IHEP-8. Both RMOFs exhibit excellent air and water stability as a result of favorable radical-radical interactions, and their long-lifetime radicals result in wide spectral absorption in the range 200-2500 nm. Gd-IHEP-7 and Gd-IHEP-8 show excellent activity toward solar-driven nitrogen fixation, with ammonia production rates of 128 and 220 μmol h-1 g-1 , respectively. Experiments and theoretical calculations indicate that both RMOFs have similar nitrogen fixation pathways. The enhanced catalytic efficiency of Gd-IHEP-8 versus Gd-IHEP-7 is attributed to intermediates stabilized by enhanced hydrogen bonding. |
| Author | Hu, Kong‐Qiu An, Shu‐Wen Zhang, Zhi‐Hui Bu, Yun‐Fei Zeng, Li‐Wen Chai, Zhi‐Fang Xu, Zhong‐Fei Lan, Jian‐Hui Yu, Ji‐Pan Shi, Wei‐Qun Mei, Lei Huang, Zhi‐Wei Kong, Xiang‐He Gibson, John K. Hu, Shu‐Xian Qiu, Peng‐Xiang |
| Author_xml | – sequence: 1 givenname: Kong‐Qiu surname: Hu fullname: Hu, Kong‐Qiu organization: Chinese Academy of Sciences – sequence: 2 givenname: Peng‐Xiang surname: Qiu fullname: Qiu, Peng‐Xiang organization: Nanjing University of Information Science and Technology – sequence: 3 givenname: Li‐Wen surname: Zeng fullname: Zeng, Li‐Wen organization: Chinese Academy of Sciences – sequence: 4 givenname: Shu‐Xian surname: Hu fullname: Hu, Shu‐Xian organization: University of Science and Technology Beijing – sequence: 5 givenname: Lei surname: Mei fullname: Mei, Lei organization: Chinese Academy of Sciences – sequence: 6 givenname: Shu‐Wen surname: An fullname: An, Shu‐Wen organization: Chinese Academy of Sciences – sequence: 7 givenname: Zhi‐Wei surname: Huang fullname: Huang, Zhi‐Wei organization: Chinese Academy of Sciences – sequence: 8 givenname: Xiang‐He surname: Kong fullname: Kong, Xiang‐He organization: Chinese Academy of Sciences – sequence: 9 givenname: Jian‐Hui surname: Lan fullname: Lan, Jian‐Hui organization: Chinese Academy of Sciences – sequence: 10 givenname: Ji‐Pan surname: Yu fullname: Yu, Ji‐Pan organization: Chinese Academy of Sciences – sequence: 11 givenname: Zhi‐Hui surname: Zhang fullname: Zhang, Zhi‐Hui organization: Changzhou University – sequence: 12 givenname: Zhong‐Fei surname: Xu fullname: Xu, Zhong‐Fei organization: University of Science and Technology Beijing – sequence: 13 givenname: John K. surname: Gibson fullname: Gibson, John K. organization: Lawrence Berkeley National Laboratory (LBNL) – sequence: 14 givenname: Zhi‐Fang surname: Chai fullname: Chai, Zhi‐Fang organization: Chinese Academy of Sciences – sequence: 15 givenname: Yun‐Fei surname: Bu fullname: Bu, Yun‐Fei organization: Nanjing University of Information Science and Technology – sequence: 16 givenname: Wei‐Qun orcidid: 0000-0001-9929-9732 surname: Shi fullname: Shi, Wei‐Qun email: shiwq@ihep.ac.cn organization: Chinese Academy of Sciences |
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| Snippet | Herein we present a new viologen‐based radical‐containing metal–organic framework (RMOF) Gd‐IHEP‐7, which upon heating in air undergoes a... Herein we present a new viologen-based radical-containing metal-organic framework (RMOF) Gd-IHEP-7, which upon heating in air undergoes a... |
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| SubjectTerms | Absorption spectra Ammonia Gadolinium Hydrogen bonding hydrogen bonds Intermediates Metal-organic frameworks Nitrogen Nitrogen fixation Nitrogenation photocatalytic nitrogen fixation radical-containing MOFs single-crystal-to-single-crystal viologen Water stability |
| Title | Solar‐Driven Nitrogen Fixation Catalyzed by Stable Radical‐Containing MOFs: Improved Efficiency Induced by a Structural Transformation |
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