Elucidating the Vibrational Fingerprint of the Flexible Metal-Organic Framework MIL-53(Al) Using a Combined Experimental/Computational Approach
In this work, mid-infrared (mid-IR), far-IR, and Raman spectra are presented for the distinct (meta)stable phases of the flexible metal-organic framework MIL-53(Al). Static density functional theory (DFT) simulations are performed, allowing for the identification of all IR-active modes, which is unp...
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| Vydané v: | Journal of physical chemistry. C Ročník 122; číslo 5; s. 2734 |
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| Hlavní autori: | , , , , , , , , |
| Médium: | Journal Article |
| Jazyk: | English |
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United States
08.02.2018
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| ISSN: | 1932-7447 |
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| Abstract | In this work, mid-infrared (mid-IR), far-IR, and Raman spectra are presented for the distinct (meta)stable phases of the flexible metal-organic framework MIL-53(Al). Static density functional theory (DFT) simulations are performed, allowing for the identification of all IR-active modes, which is unprecedented in the low-frequency region. A unique vibrational fingerprint is revealed, resulting from aluminum-oxide backbone stretching modes, which can be used to clearly distinguish the IR spectra of the closed- and large-pore phases. Furthermore, molecular dynamics simulations based on a DFT description of the potential energy surface enable determination of the theoretical Raman spectrum of the closed- and large-pore phases for the first time. An excellent correspondence between theory and experiment is observed. Both the low-frequency IR and Raman spectra show major differences in vibrational modes between the closed- and large-pore phases, indicating changes in lattice dynamics between the two structures. In addition, several collective modes related to the breathing mechanism in MIL-53(Al) are identified. In particular, we rationalize the importance of the trampoline-like motion of the linker for the phase transition. |
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| AbstractList | In this work, mid-infrared (mid-IR), far-IR, and Raman spectra are presented for the distinct (meta)stable phases of the flexible metal-organic framework MIL-53(Al). Static density functional theory (DFT) simulations are performed, allowing for the identification of all IR-active modes, which is unprecedented in the low-frequency region. A unique vibrational fingerprint is revealed, resulting from aluminum-oxide backbone stretching modes, which can be used to clearly distinguish the IR spectra of the closed- and large-pore phases. Furthermore, molecular dynamics simulations based on a DFT description of the potential energy surface enable determination of the theoretical Raman spectrum of the closed- and large-pore phases for the first time. An excellent correspondence between theory and experiment is observed. Both the low-frequency IR and Raman spectra show major differences in vibrational modes between the closed- and large-pore phases, indicating changes in lattice dynamics between the two structures. In addition, several collective modes related to the breathing mechanism in MIL-53(Al) are identified. In particular, we rationalize the importance of the trampoline-like motion of the linker for the phase transition. In this work, mid-infrared (mid-IR), far-IR, and Raman spectra are presented for the distinct (meta)stable phases of the flexible metal-organic framework MIL-53(Al). Static density functional theory (DFT) simulations are performed, allowing for the identification of all IR-active modes, which is unprecedented in the low-frequency region. A unique vibrational fingerprint is revealed, resulting from aluminum-oxide backbone stretching modes, which can be used to clearly distinguish the IR spectra of the closed- and large-pore phases. Furthermore, molecular dynamics simulations based on a DFT description of the potential energy surface enable determination of the theoretical Raman spectrum of the closed- and large-pore phases for the first time. An excellent correspondence between theory and experiment is observed. Both the low-frequency IR and Raman spectra show major differences in vibrational modes between the closed- and large-pore phases, indicating changes in lattice dynamics between the two structures. In addition, several collective modes related to the breathing mechanism in MIL-53(Al) are identified. In particular, we rationalize the importance of the trampoline-like motion of the linker for the phase transition.In this work, mid-infrared (mid-IR), far-IR, and Raman spectra are presented for the distinct (meta)stable phases of the flexible metal-organic framework MIL-53(Al). Static density functional theory (DFT) simulations are performed, allowing for the identification of all IR-active modes, which is unprecedented in the low-frequency region. A unique vibrational fingerprint is revealed, resulting from aluminum-oxide backbone stretching modes, which can be used to clearly distinguish the IR spectra of the closed- and large-pore phases. Furthermore, molecular dynamics simulations based on a DFT description of the potential energy surface enable determination of the theoretical Raman spectrum of the closed- and large-pore phases for the first time. An excellent correspondence between theory and experiment is observed. Both the low-frequency IR and Raman spectra show major differences in vibrational modes between the closed- and large-pore phases, indicating changes in lattice dynamics between the two structures. In addition, several collective modes related to the breathing mechanism in MIL-53(Al) are identified. In particular, we rationalize the importance of the trampoline-like motion of the linker for the phase transition. |
| Author | Depauw, Hannes Wieme, Jelle Vrielinck, Henk Nevjestić, Irena Van Der Voort, Pascal Rogge, Sven M J Hoffman, Alexander E J Vanduyfhuys, Louis Van Speybroeck, Veronique |
| Author_xml | – sequence: 1 givenname: Alexander E J surname: Hoffman fullname: Hoffman, Alexander E J organization: Department of Solid State Sciences, Ghent University, Krijgslaan 281-S1, 9000 Ghent, Belgium – sequence: 2 givenname: Louis surname: Vanduyfhuys fullname: Vanduyfhuys, Louis organization: Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde, Belgium – sequence: 3 givenname: Irena surname: Nevjestić fullname: Nevjestić, Irena organization: Department of Solid State Sciences, Ghent University, Krijgslaan 281-S1, 9000 Ghent, Belgium – sequence: 4 givenname: Jelle surname: Wieme fullname: Wieme, Jelle organization: Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde, Belgium – sequence: 5 givenname: Sven M J surname: Rogge fullname: Rogge, Sven M J organization: Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde, Belgium – sequence: 6 givenname: Hannes surname: Depauw fullname: Depauw, Hannes organization: Center for Ordered Materials, Organometallics and Catalysis, Ghent University, Krijgslaan 281-S3, 9000 Ghent, Belgium – sequence: 7 givenname: Pascal surname: Van Der Voort fullname: Van Der Voort, Pascal organization: Center for Ordered Materials, Organometallics and Catalysis, Ghent University, Krijgslaan 281-S3, 9000 Ghent, Belgium – sequence: 8 givenname: Henk surname: Vrielinck fullname: Vrielinck, Henk organization: Department of Solid State Sciences, Ghent University, Krijgslaan 281-S1, 9000 Ghent, Belgium – sequence: 9 givenname: Veronique surname: Van Speybroeck fullname: Van Speybroeck, Veronique organization: Center for Molecular Modeling, Ghent University, Technologiepark 903, 9052 Zwijnaarde, Belgium |
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