Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J51) Nonanuclear Zr-Oxocarboxylate Clusters

Wei Gong; Hadi Arman; Zhijie Chen; Yi Xie; Florencia A. Son; Hui Cui; Xinfa Chen; Yanshu Shi; Yan Liu; Banglin Chen; Omar K. Farha; Yong Cui

doi:10.1021/jacs.0c11881

Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J₅₁) Nonanuclear Zr-Oxocarboxylate Clusters

Wei Gong, Hadi Arman, Zhijie Chen, Yi Xie, Florencia A. Son, Hui Cui, Xinfa Chen, Yanshu Shi, Yan Liu, Banglin Chen, Omar K. Farha, Yong Cui^*

^*Corresponding author for this work

Chemistry

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

15 Scopus citations

Abstract

The quest for new and unique polynuclear metal-oxocarboxylate clusters has led to a continual boom of highly connected and robust metal-organic frameworks (MOFs) with intriguing properties. In this work, by virtue of a highly specific coordination-driven cluster rearrangement process of a presynthesized trinuclear zirconocene-based tripodal metallo-pyridine ligand, we realized the preparation of the first two 2D heterometallic MOFs incorporating unprecedented Johnson-type (J51) nonanuclear Zr-oxocarboxylate clusters, as unambiguously uncovered by single-crystal X-ray crystallography. The resultant two charged frameworks feature counteranion-dependent 3,6-c kgd (JMOF-1) and 3,12-c 3,12L4 (JMOF-2) nets that are formed by octahedral and hexagonal prismatic Zr9 molecular building blocks (MBBs), respectively. In addition, JMOF-2 shows promise for the purification of acetylene from CO2 and C2H4, with IAST selectivities of about 12 and 8, respectively, at 298 K and 1 bar, as well as remarkable iodine capture capacity of up to 2.4 g g-1.

Original language	English (US)
Pages (from-to)	657-663
Number of pages	7
Journal	Journal of the American Chemical Society
Volume	143
Issue number	2
DOIs	https://doi.org/10.1021/jacs.0c11881
State	Published - Jan 20 2021

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.0c11881

Cite this

Gong, W., Arman, H., Chen, Z., Xie, Y., Son, F. A., Cui, H., Chen, X., Shi, Y., Liu, Y., Chen, B., Farha, O. K., & Cui, Y. (2021). Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J₅₁) Nonanuclear Zr-Oxocarboxylate Clusters. Journal of the American Chemical Society, 143(2), 657-663. https://doi.org/10.1021/jacs.0c11881

@article{aa1afc0a7d984fcaaa6636b1674a3e0d,

title = "Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J51) Nonanuclear Zr-Oxocarboxylate Clusters",

abstract = "The quest for new and unique polynuclear metal-oxocarboxylate clusters has led to a continual boom of highly connected and robust metal-organic frameworks (MOFs) with intriguing properties. In this work, by virtue of a highly specific coordination-driven cluster rearrangement process of a presynthesized trinuclear zirconocene-based tripodal metallo-pyridine ligand, we realized the preparation of the first two 2D heterometallic MOFs incorporating unprecedented Johnson-type (J51) nonanuclear Zr-oxocarboxylate clusters, as unambiguously uncovered by single-crystal X-ray crystallography. The resultant two charged frameworks feature counteranion-dependent 3,6-c kgd (JMOF-1) and 3,12-c 3,12L4 (JMOF-2) nets that are formed by octahedral and hexagonal prismatic Zr9 molecular building blocks (MBBs), respectively. In addition, JMOF-2 shows promise for the purification of acetylene from CO2 and C2H4, with IAST selectivities of about 12 and 8, respectively, at 298 K and 1 bar, as well as remarkable iodine capture capacity of up to 2.4 g g-1.",

author = "Wei Gong and Hadi Arman and Zhijie Chen and Yi Xie and Son, {Florencia A.} and Hui Cui and Xinfa Chen and Yanshu Shi and Yan Liu and Banglin Chen and Farha, {Omar K.} and Yong Cui",

note = "Funding Information: This work was financially supported by the National Science Foundation of China (Grants 21620102001, 91856204, 91956124, and 21875136), the National Key Basic Research Program of China (2016YFA0203400), Key Project of Basic Research of Shanghai (18JC1413200 and 19JC1412600), the Shanghai Rising-Star Program (19QA1404300), and the China Postdoctoral Science Foundation (2019M661482). O.K.F. gratefully acknowledges research support from the U.S. Department of Energy{\textquoteright}s Office of Energy Efficiency and Renewable Energy (EERE) under Award DE-EE0008816. F.A.S. is supported by the Department of Defense (DoD) through the National Defense Science & Engineering Graduate (NDSEG) Fellowship Program. Publisher Copyright: {\textcopyright} 2021 American Chemical Society.",

year = "2021",

month = jan,

day = "20",

doi = "10.1021/jacs.0c11881",

language = "English (US)",

volume = "143",

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Gong, W, Arman, H, Chen, Z, Xie, Y, Son, FA, Cui, H, Chen, X, Shi, Y, Liu, Y, Chen, B, Farha, OK & Cui, Y 2021, 'Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J₅₁) Nonanuclear Zr-Oxocarboxylate Clusters', Journal of the American Chemical Society, vol. 143, no. 2, pp. 657-663. https://doi.org/10.1021/jacs.0c11881

Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J₅₁) Nonanuclear Zr-Oxocarboxylate Clusters. / Gong, Wei; Arman, Hadi; Chen, Zhijie et al.
In: Journal of the American Chemical Society, Vol. 143, No. 2, 20.01.2021, p. 657-663.

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

TY - JOUR

T1 - Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J51) Nonanuclear Zr-Oxocarboxylate Clusters

AU - Gong, Wei

AU - Arman, Hadi

AU - Chen, Zhijie

AU - Xie, Yi

AU - Son, Florencia A.

AU - Cui, Hui

AU - Chen, Xinfa

AU - Shi, Yanshu

AU - Liu, Yan

AU - Chen, Banglin

AU - Farha, Omar K.

AU - Cui, Yong

N1 - Funding Information: This work was financially supported by the National Science Foundation of China (Grants 21620102001, 91856204, 91956124, and 21875136), the National Key Basic Research Program of China (2016YFA0203400), Key Project of Basic Research of Shanghai (18JC1413200 and 19JC1412600), the Shanghai Rising-Star Program (19QA1404300), and the China Postdoctoral Science Foundation (2019M661482). O.K.F. gratefully acknowledges research support from the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under Award DE-EE0008816. F.A.S. is supported by the Department of Defense (DoD) through the National Defense Science & Engineering Graduate (NDSEG) Fellowship Program. Publisher Copyright: © 2021 American Chemical Society.

PY - 2021/1/20

Y1 - 2021/1/20

N2 - The quest for new and unique polynuclear metal-oxocarboxylate clusters has led to a continual boom of highly connected and robust metal-organic frameworks (MOFs) with intriguing properties. In this work, by virtue of a highly specific coordination-driven cluster rearrangement process of a presynthesized trinuclear zirconocene-based tripodal metallo-pyridine ligand, we realized the preparation of the first two 2D heterometallic MOFs incorporating unprecedented Johnson-type (J51) nonanuclear Zr-oxocarboxylate clusters, as unambiguously uncovered by single-crystal X-ray crystallography. The resultant two charged frameworks feature counteranion-dependent 3,6-c kgd (JMOF-1) and 3,12-c 3,12L4 (JMOF-2) nets that are formed by octahedral and hexagonal prismatic Zr9 molecular building blocks (MBBs), respectively. In addition, JMOF-2 shows promise for the purification of acetylene from CO2 and C2H4, with IAST selectivities of about 12 and 8, respectively, at 298 K and 1 bar, as well as remarkable iodine capture capacity of up to 2.4 g g-1.

AB - The quest for new and unique polynuclear metal-oxocarboxylate clusters has led to a continual boom of highly connected and robust metal-organic frameworks (MOFs) with intriguing properties. In this work, by virtue of a highly specific coordination-driven cluster rearrangement process of a presynthesized trinuclear zirconocene-based tripodal metallo-pyridine ligand, we realized the preparation of the first two 2D heterometallic MOFs incorporating unprecedented Johnson-type (J51) nonanuclear Zr-oxocarboxylate clusters, as unambiguously uncovered by single-crystal X-ray crystallography. The resultant two charged frameworks feature counteranion-dependent 3,6-c kgd (JMOF-1) and 3,12-c 3,12L4 (JMOF-2) nets that are formed by octahedral and hexagonal prismatic Zr9 molecular building blocks (MBBs), respectively. In addition, JMOF-2 shows promise for the purification of acetylene from CO2 and C2H4, with IAST selectivities of about 12 and 8, respectively, at 298 K and 1 bar, as well as remarkable iodine capture capacity of up to 2.4 g g-1.

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Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J₅₁) Nonanuclear Zr-Oxocarboxylate Clusters

Abstract

ASJC Scopus subject areas

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CCDC 2048489: Experimental Crystal Structure Determination

CCDC 2048493: Experimental Crystal Structure Determination

CCDC 2048492: Experimental Crystal Structure Determination

Cite this

Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J51) Nonanuclear Zr-Oxocarboxylate Clusters

Abstract

ASJC Scopus subject areas

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Datasets

CCDC 2048489: Experimental Crystal Structure Determination

CCDC 2048493: Experimental Crystal Structure Determination

CCDC 2048492: Experimental Crystal Structure Determination

Cite this

Highly Specific Coordination-Driven Self-Assembly of 2D Heterometallic Metal-Organic Frameworks with Unprecedented Johnson-type (J₅₁) Nonanuclear Zr-Oxocarboxylate Clusters