Switched “On” Transient Fluorescence Output from a Pulsed-Fuel Molecular Ratchet

Baluna, Andrei S.; Dommaschk, Marcel; Groh, Burkhard; Kassem, Salma; Leigh, David A.; Tetlow, Daniel J.; Thomas, Dean; Varela López, Loli

doi:10.1021/jacs.3c11290

“…Artificial MIMs have been created using different chemical strategies. , Such strategies can be broadly divided into two categories, one where the interlocked structures are formed under kinetic control , and the second category where the structures are formed through thermodynamic control using dynamic bonds. , The first synthetic strategy suffers from low yields, and hence the second is generally favored. Using the dynamic bonding approach, multiple MIMs have been created with different topologies, , such as rotaxanes, − knots, − rings, ravels, , and catenanes. − …”

Section: Introductionmentioning

confidence: 99%

Mechanically Interlocked Water-Soluble Pd₆ Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules

Chakraborty,

Pradhan,

Clegg

et al. 2024

Inorg. Chem.

0

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Research on the synthesis of catenated cages has been a growing field of interest in the past few years. While multiple types of catenated cages with different structures have been synthesized, the application of such systems has been much less explored. Specifically, the use of catenated cages in the separation of industrially relevant molecules that are present in coal tar has not been explored before. Herein, we demonstrate the use of a newly synthesized interlocked cage 1 [C 184 H 240 N 76 O 48 Pd 6 ] (M 6 L 4 ), formed through the self-assembly of ligand L.HNO 3 (tris(4-(1H-imidazole-1yl)benzylidene)hydrazine-1-carbohydrazonhydrazide) with acceptor cis-[(tmchda)Pd-(NO 3 ) 2 ] [tmchda = ±N,N,N′,N′-tetramethylcyclohexane-1,2-diamine] (M). The interlocked cage 1 was able to separate the isomers (anthracene and phenanthrene) using a simple solvent extraction technique. Using the same technique, the much more difficult separation of structurally and physiochemically similar compounds acenaphthene and acenaphthylene was performed for the first time with 1 as the host. Other noninterlocked hexanuclear Pd 6 cages having a wider cavity proved inefficient for such separation, demonstrating the uniqueness of the interlocked cage 1 for such challenging separation.

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Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

Borsley,

Leigh,

Roberts

2024

Angewandte Chemie

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In recent years ratchet mechanisms have transformed the understanding and design of stochastic molecular systems—biological, chemical and physical—in a move away from the mechanical macroscopic analogies that dominated thinking regarding molecular dynamics in the 1990s and early 2000s (e.g. pistons, springs, etc), to the more scale‐relevant concepts that underpin out‐of‐equilibrium research in the molecular sciences today. Ratcheting has established molecular nanotechnology as a research frontier for energy transduction and metabolism, and has enabled the reverse engineering of biomolecular machinery, delivering insights into how molecules ‘walk’ and track‐based synthesizers operate, how the acceleration of chemical reactions enables energy to be transduced by catalysts, and how dynamic (supra)molecular systems can be driven away from equilibrium. The recognition of molecular ratchet mechanisms in biology, and their invention in synthetic systems, is proving significant in areas as diverse as supramolecular chemistry, systems chemistry, dynamic covalent chemistry, DNA nanotechnology, polymer and materials science, molecular biology, heterogeneous catalysis, endergonic synthesis, and many other branches of chemical science. Put simply, ratchet mechanisms give chemistry direction. Kinetic asymmetry, quantified by the outcome of ratcheting, is the dynamic counterpart of structural asymmetry (i.e. chirality). Given the ubiquity of ratchet mechanisms, it is surely just as fundamentally important.

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Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

Borsley,

Leigh,

Roberts

2024

Angew Chem Int Ed

Self Cite

6

0

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In recent years ratchet mechanisms have transformed the understanding and design of stochastic molecular systems—biological, chemical and physical—in a move away from the mechanical macroscopic analogies that dominated thinking regarding molecular dynamics in the 1990s and early 2000s (e.g. pistons, springs, etc), to the more scale‐relevant concepts that underpin out‐of‐equilibrium research in the molecular sciences today. Ratcheting has established molecular nanotechnology as a research frontier for energy transduction and metabolism, and has enabled the reverse engineering of biomolecular machinery, delivering insights into how molecules ‘walk’ and track‐based synthesizers operate, how the acceleration of chemical reactions enables energy to be transduced by catalysts, and how dynamic (supra)molecular systems can be driven away from equilibrium. The recognition of molecular ratchet mechanisms in biology, and their invention in synthetic systems, is proving significant in areas as diverse as supramolecular chemistry, systems chemistry, dynamic covalent chemistry, DNA nanotechnology, polymer and materials science, molecular biology, heterogeneous catalysis, endergonic synthesis, and many other branches of chemical science. Put simply, ratchet mechanisms give chemistry direction. Kinetic asymmetry, quantified by the outcome of ratcheting, is the dynamic counterpart of structural asymmetry (i.e. chirality). Given the ubiquity of ratchet mechanisms, it is surely just as fundamentally important.

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Switched “On” Transient Fluorescence Output from a Pulsed-Fuel Molecular Ratchet

Cited by 4 publications

References 75 publications

Mechanically Interlocked Water-Soluble Pd₆ Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules

Mechanically Interlocked Water-Soluble Pd₆ Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

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Switched “On” Transient Fluorescence Output from a Pulsed-Fuel Molecular Ratchet

Cited by 4 publications

References 75 publications

Mechanically Interlocked Water-Soluble Pd6 Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules

Mechanically Interlocked Water-Soluble Pd6 Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

Molecular Ratchets and Kinetic Asymmetry: Giving Chemistry Direction

Contact Info

Product

Resources

About

Mechanically Interlocked Water-Soluble Pd₆ Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules

Mechanically Interlocked Water-Soluble Pd₆ Host for the Selective Separation of Coal Tar-Based Planar Aromatic Molecules