Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101

Petra Ágota Szilágyi; Ingrid Weinrauch; Hyunchul Oh; Michael Hirscher; Jana Juan-Alcañiz; Pablo Serra-Crespo; Moreno De Respinis; Bartek Jacek Trześniewski; Freek Kapteijn; Hans Geerlings; Jorge Gascon; Bernard Dam; Anna Grzech; Roel Van De Krol

doi:10.1021/jp5050628

Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101

Petra Ágota Szilágyi^*, Ingrid Weinrauch, Hyunchul Oh, Michael Hirscher, Jana Juan-Alcañiz, Pablo Serra-Crespo, Moreno De Respinis, Bartek Jacek Trześniewski, Freek Kapteijn, Hans Geerlings, Jorge Gascon, Bernard Dam, Anna Grzech, Roel Van De Krol

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

22 Scopus citations

Abstract

Functionalization of metal-organic frameworks results in higher hydrogen uptakes owing to stronger hydrogen-host interactions. However, it has not been studied whether a given functional group acts on existing adsorption sites (linker or metal) or introduces new ones. In this work, the effect of two types of functional groups on MIL-101 (Cr) is analyzed. Thermal-desorption spectroscopy reveals that the -Br ligand increases the secondary building unit's hydrogen affinity, while the -NH₂ functional group introduces new hydrogen adsorption sites. In addition, a subsequent introduction of -Br and -NH₂ ligands on the linker results in the highest hydrogen-store interaction energy on the cationic nodes. The latter is attributed to a push-and-pull effect of the linkers.

Original language	English (US)
Pages (from-to)	19572-19579
Number of pages	8
Journal	JOURNAL OF PHYSICAL CHEMISTRY C
Volume	118
Issue number	34
DOIs	https://doi.org/10.1021/jp5050628
State	Published - Aug 28 2014
Externally published	Yes

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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10.1021/jp5050628

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Szilágyi, P. Á., Weinrauch, I., Oh, H., Hirscher, M., Juan-Alcañiz, J., Serra-Crespo, P., De Respinis, M., Trześniewski, B. J., Kapteijn, F., Geerlings, H., Gascon, J., Dam, B., Grzech, A., & Van De Krol, R. (2014). Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101. JOURNAL OF PHYSICAL CHEMISTRY C, 118(34), 19572-19579. https://doi.org/10.1021/jp5050628

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title = "Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101",

abstract = "Functionalization of metal-organic frameworks results in higher hydrogen uptakes owing to stronger hydrogen-host interactions. However, it has not been studied whether a given functional group acts on existing adsorption sites (linker or metal) or introduces new ones. In this work, the effect of two types of functional groups on MIL-101 (Cr) is analyzed. Thermal-desorption spectroscopy reveals that the -Br ligand increases the secondary building unit's hydrogen affinity, while the -NH2 functional group introduces new hydrogen adsorption sites. In addition, a subsequent introduction of -Br and -NH2 ligands on the linker results in the highest hydrogen-store interaction energy on the cationic nodes. The latter is attributed to a push-and-pull effect of the linkers.",

author = "Szil{\'a}gyi, {Petra {\'A}gota} and Ingrid Weinrauch and Hyunchul Oh and Michael Hirscher and Jana Juan-Alca{\~n}iz and Pablo Serra-Crespo and {De Respinis}, Moreno and Trze{\'s}niewski, {Bartek Jacek} and Freek Kapteijn and Hans Geerlings and Jorge Gascon and Bernard Dam and Anna Grzech and {Van De Krol}, Roel",

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Szilágyi, PÁ, Weinrauch, I, Oh, H, Hirscher, M, Juan-Alcañiz, J, Serra-Crespo, P, De Respinis, M, Trześniewski, BJ, Kapteijn, F, Geerlings, H, Gascon, J, Dam, B, Grzech, A & Van De Krol, R 2014, 'Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101', JOURNAL OF PHYSICAL CHEMISTRY C, vol. 118, no. 34, pp. 19572-19579. https://doi.org/10.1021/jp5050628

TY - JOUR

T1 - Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101

AU - Szilágyi, Petra Ágota

AU - Weinrauch, Ingrid

AU - Oh, Hyunchul

AU - Hirscher, Michael

AU - Juan-Alcañiz, Jana

AU - Serra-Crespo, Pablo

AU - De Respinis, Moreno

AU - Trześniewski, Bartek Jacek

AU - Kapteijn, Freek

AU - Geerlings, Hans

AU - Gascon, Jorge

AU - Dam, Bernard

AU - Grzech, Anna

AU - Van De Krol, Roel

PY - 2014/8/28

Y1 - 2014/8/28

N2 - Functionalization of metal-organic frameworks results in higher hydrogen uptakes owing to stronger hydrogen-host interactions. However, it has not been studied whether a given functional group acts on existing adsorption sites (linker or metal) or introduces new ones. In this work, the effect of two types of functional groups on MIL-101 (Cr) is analyzed. Thermal-desorption spectroscopy reveals that the -Br ligand increases the secondary building unit's hydrogen affinity, while the -NH2 functional group introduces new hydrogen adsorption sites. In addition, a subsequent introduction of -Br and -NH2 ligands on the linker results in the highest hydrogen-store interaction energy on the cationic nodes. The latter is attributed to a push-and-pull effect of the linkers.

AB - Functionalization of metal-organic frameworks results in higher hydrogen uptakes owing to stronger hydrogen-host interactions. However, it has not been studied whether a given functional group acts on existing adsorption sites (linker or metal) or introduces new ones. In this work, the effect of two types of functional groups on MIL-101 (Cr) is analyzed. Thermal-desorption spectroscopy reveals that the -Br ligand increases the secondary building unit's hydrogen affinity, while the -NH2 functional group introduces new hydrogen adsorption sites. In addition, a subsequent introduction of -Br and -NH2 ligands on the linker results in the highest hydrogen-store interaction energy on the cationic nodes. The latter is attributed to a push-and-pull effect of the linkers.

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JF - JOURNAL OF PHYSICAL CHEMISTRY C

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Interplay of linker functionalization and hydrogen adsorption in the metal-organic framework MIL-101

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