Balancing Ligand Flexibility versus Rigidity for the Stepwise Self-Assembly of M12L24 via M6L12 Metal–Organic Cages

C.-L. Liu; E.O. Bobylev; Y. Fu; D.A. Poole; K. Robeyns; C.-A. Fustin; Y. Garcia; J.N.H. Reek; M.L. Singleton

doi:10.1002/chem.202001399

Balancing Ligand Flexibility versus Rigidity for the Stepwise Self-Assembly of M12L24 via M6L12 Metal–Organic Cages

C.-L. Liu, E.O. Bobylev, Y. Fu, D.A. Poole, K. Robeyns, C.-A. Fustin, Y. Garcia, J.N.H. Reek, M.L. Singleton

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

© 2020 Wiley-VCH GmbHNon-covalent interactions are important for directing protein folding across multiple intermediates and can even provide access to multiple stable structures with different properties and functions. Herein, we describe an approach for mimicking this behavior in the self-assembly of metal–organic cages. Two ligands, the bend angles of which are controlled by non-covalent interactions and one ligand lacking the above-mentioned interactions, were synthesized and used for self-assembly with Pd2+. As these weak interactions are easily broken, the bend angles have a controlled flexibility giving access to M2(L1)4, M6(L2)12, and M12(L2)24 cages. By controlling the self-assembly conditions this process can be directed in a stepwise fashion. Additionally, the multiple endohedral hydrogen-bonding sites on the ligand were found to play a role in the binding and discrimination of neutral guests.

Original language	English
Pages (from-to)	11960-11965
Journal	Chemistry - A European Journal
Volume	26
Issue number	52
DOIs	https://doi.org/10.1002/chem.202001399
Publication status	Published - 16 Sept 2020
Externally published	Yes

Funding

This work was supported in part through the Concerted Research Action (ARC16/21‐074). C.‐L.L. and Y.F were supported by fellowships from the China Scholarship Council. Computational resources have been provided by the supercomputing facilities of the Université catholique de Louvain (CISM/UCL) and the Consortium des équipements de Calcul Intensif en Fédération Wallonie Bruxelles (CPCI) funded by the Fond de la Recherche Scientifique de Belgique (F.R.S.‐FNRS) under convention 2.5020.11. We also thank Dr. G. Barozzino for help with NMR measurements.

Funders	Funder number
CISM
CPCI
Concerted Research Action	ARC16/21‐074
Consortium des équipements de Calcul Intensif en Fédération Wallonie Bruxelles
F.R.S.‐FNRS
Fond de la Recherche Scientifique de Belgique
Université Catholique de Louvain
China Scholarship Council
Université Catholique de Louvain

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title = "Balancing Ligand Flexibility versus Rigidity for the Stepwise Self-Assembly of M12L24 via M6L12 Metal–Organic Cages",

abstract = "{\textcopyright} 2020 Wiley-VCH GmbHNon-covalent interactions are important for directing protein folding across multiple intermediates and can even provide access to multiple stable structures with different properties and functions. Herein, we describe an approach for mimicking this behavior in the self-assembly of metal–organic cages. Two ligands, the bend angles of which are controlled by non-covalent interactions and one ligand lacking the above-mentioned interactions, were synthesized and used for self-assembly with Pd2+. As these weak interactions are easily broken, the bend angles have a controlled flexibility giving access to M2(L1)4, M6(L2)12, and M12(L2)24 cages. By controlling the self-assembly conditions this process can be directed in a stepwise fashion. Additionally, the multiple endohedral hydrogen-bonding sites on the ligand were found to play a role in the binding and discrimination of neutral guests.",

author = "C.-L. Liu and E.O. Bobylev and Y. Fu and D.A. Poole and K. Robeyns and C.-A. Fustin and Y. Garcia and J.N.H. Reek and M.L. Singleton",

year = "2020",

month = sep,

day = "16",

doi = "10.1002/chem.202001399",

language = "English",

volume = "26",

pages = "11960--11965",

journal = "Chemistry - A European Journal",

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T1 - Balancing Ligand Flexibility versus Rigidity for the Stepwise Self-Assembly of M12L24 via M6L12 Metal–Organic Cages

AU - Liu, C.-L.

AU - Bobylev, E.O.

AU - Fu, Y.

AU - Poole, D.A.

AU - Robeyns, K.

AU - Fustin, C.-A.

AU - Garcia, Y.

AU - Reek, J.N.H.

AU - Singleton, M.L.

PY - 2020/9/16

Y1 - 2020/9/16

N2 - © 2020 Wiley-VCH GmbHNon-covalent interactions are important for directing protein folding across multiple intermediates and can even provide access to multiple stable structures with different properties and functions. Herein, we describe an approach for mimicking this behavior in the self-assembly of metal–organic cages. Two ligands, the bend angles of which are controlled by non-covalent interactions and one ligand lacking the above-mentioned interactions, were synthesized and used for self-assembly with Pd2+. As these weak interactions are easily broken, the bend angles have a controlled flexibility giving access to M2(L1)4, M6(L2)12, and M12(L2)24 cages. By controlling the self-assembly conditions this process can be directed in a stepwise fashion. Additionally, the multiple endohedral hydrogen-bonding sites on the ligand were found to play a role in the binding and discrimination of neutral guests.

AB - © 2020 Wiley-VCH GmbHNon-covalent interactions are important for directing protein folding across multiple intermediates and can even provide access to multiple stable structures with different properties and functions. Herein, we describe an approach for mimicking this behavior in the self-assembly of metal–organic cages. Two ligands, the bend angles of which are controlled by non-covalent interactions and one ligand lacking the above-mentioned interactions, were synthesized and used for self-assembly with Pd2+. As these weak interactions are easily broken, the bend angles have a controlled flexibility giving access to M2(L1)4, M6(L2)12, and M12(L2)24 cages. By controlling the self-assembly conditions this process can be directed in a stepwise fashion. Additionally, the multiple endohedral hydrogen-bonding sites on the ligand were found to play a role in the binding and discrimination of neutral guests.

U2 - 10.1002/chem.202001399

DO - 10.1002/chem.202001399

M3 - Article

SN - 0947-6539

VL - 26

SP - 11960

EP - 11965

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

IS - 52

ER -

Balancing Ligand Flexibility versus Rigidity for the Stepwise Self-Assembly of M12L24 via M6L12 Metal–Organic Cages

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