Self-assembly of triangular metallomacrocycles using unsymmetrical bisterpyridine ligands: isomer differentiation via TWIM mass spectrometry

2015 ◽  
Vol 44 (11) ◽  
pp. 5139-5145 ◽  
Author(s):  
Yen-Peng Liang ◽  
Yun-Jui He ◽  
Yin-Hsuan Lee ◽  
Yi-Tsu Chan
Keyword(s):  
Mass Spectrometry ◽  
Self Assembly ◽  
Isomer Differentiation

A mixture of isomeric metallotriangles, assembled from unsymmetrical bisterpyridine ligands and ZnII ions, was successfully differentiated with MS2 TWIM MS.

Click Synthesis of Shape-Persistent Azodendrimers and their Orthogonal Self-Assembly to Nanofibres

2018 ◽  
Vol 71 (6) ◽  
pp. 463 ◽  
Author(s):  
Tamer El Malah ◽  
Hany F. Nour
Keyword(s):  
Electron Microscopy ◽  
Mass Spectrometry ◽  
Self Assembly ◽  
Molecular Structures ◽  
Side Chain ◽  
Spectroscopic Techniques ◽  
Molecular Weights ◽  
Transmission Electron ◽  
Click Synthesis ◽  
Scanning Electron

The copper(i)-catalyzed azide–alkyne cycloaddition (CuAAC) reaction has been efficiently utilized to synthesize a series of dendrons with amino functionalities. The aminodendrons successfully underwent azodimerization to furnish a series of pyridyl- and phenyl-based azodendrimers with peripheral alkyl or ether side chain substituents. The molecular structures of the azodendrimers were fully assigned using different spectroscopic techniques, such as 1H NMR and 13C NMR, and the molecular weights were determined using MALDI-TOF mass spectrometry. The molecular self-assembly of the azodendrimers was investigated by scanning electron microscopy and transmission electron microscopy, which revealed the formation of highly ordered and uniform self-assembled nanofibres.

scholarly journals Molecular basis for chirality-regulated Aβ self-assembly and receptor recognition revealed by ion mobility-mass spectrometry

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Gongyu Li ◽  
Kellen DeLaney ◽  
Lingjun Li
Keyword(s):  
Mass Spectrometry ◽  
Ion Mobility ◽  
Self Assembly ◽  
Molecular Basis ◽  
Drug Targets ◽  
Molecular Evidence ◽  
Ion Mobility Mass Spectrometry ◽  
Epitope Region ◽  
Receptor Recognition ◽  
Chiral Effects

Abstract Despite extensive efforts on probing the mechanism of Alzheimer’s disease (AD) and enormous investments into AD drug development, the lack of effective disease-modifying therapeutics and the complexity of the AD pathogenesis process suggest a great need for further insights into alternative AD drug targets. Herein, we focus on the chiral effects of truncated amyloid beta (Aβ) and offer further structural and molecular evidence for epitope region-specific, chirality-regulated Aβ fragment self-assembly and its potential impact on receptor-recognition. A multidimensional ion mobility-mass spectrometry (IM-MS) analytical platform and in-solution kinetics analysis reveal the comprehensive structural and molecular basis for differential Aβ fragment chiral chemistry, including the differential and cooperative roles of chiral Aβ N-terminal and C-terminal fragments in receptor recognition. Our method is applicable to many other systems and the results may shed light on the potential development of novel AD therapeutic strategies based on targeting the D-isomerized Aβ, rather than natural L-Aβ.

Self-assembly of a nonanuclear NiII cluster via atmospheric CO2 fixation: synthesis, structure, collision-induced dissociation mass spectrometry and magnetic property

2020 ◽  
Vol 49 (31) ◽  
pp. 10977-10982
Author(s):  
Xue-Fei Tian ◽  
Bao-Qian Ji ◽  
Lei Feng ◽  
Kai Sheng ◽  
Yan-Min Su ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Magnetic Property ◽  
Self Assembly ◽  
Co2 Fixation ◽  
Mixed Ligand ◽  
Atmospheric Co2 ◽  
Collision Induced Dissociation

The atmospheric CO2 was spontaneously fixed into a novel nonanuclear Ni(ii) cluster which has been easily and successfully constructed through a mixed-ligand approach.

Nuclear magnetic resonance and mass spectrometry studies of 2′,3′,5′-O-triacetylguanosine self-assembly in the presence of alkaline earth metal ions (Ca2+, Sr2+, Ba2+)

2011 ◽  
Vol 89 (7) ◽  
pp. 835-844 ◽  
Author(s):  
Irene C.M. Kwan ◽  
Yi-Min She ◽  
Gang Wu
Keyword(s):  
Mass Spectrometry ◽  
Nuclear Magnetic Resonance ◽  
Magnetic Resonance ◽  
Metal Ions ◽  
Self Assembly ◽  
Alkaline Earth ◽  
Earth Metal ◽  
Alkaline Earth Metal ◽  
Alkaline Earth Metal Ions ◽  
Nuclear Magnetic

We report structural determination of cation-templated self-assembly of a guanosine derivative, 2′,3′,5′-O-triacetylguanosine (TAG), in the presence of three alkaline earth metal ions (Ca2+, Sr2+, and Ba2+) in CDCl3. Using a combination of nuclear magnetic resonance (NMR) and electrospray ionization mass spectrometry (ESI-MS) methods, we have found that TAG molecules form discrete octamers in the form of [TAG]8M2+ (M2+ = Ca2+, Sr2+, and Ba2+), which is composed of two G-quartets and a sandwiched metal ion. We have determined the ability of the three alkaline earth metal ions to promote TAG self-assembly (relative binding affinity) to be Sr2+ ≫ Ba2+ > Ca2+. More importantly, we have used two-dimensional (2D) NMR methods to determine the structural details of [TAG]8Sr2+. In particular, we found that each octamer consists of an all-anti G-quartet stacking on top of an all-syn G-quartet in a tail-to-head fashion with a twist angle of 45° between the two G-quartets. This TAG octamer structure represents a unique case quite different from other lipophilic guanosine octamers reported in the literature.

scholarly journals Reaction Monitoring and Structural Characterisation of Coordination Driven Self-Assembled Systems by Ion Mobility-Mass Spectrometry

2021 ◽  
Vol 9 ◽  
Author(s):  
Oscar H. Lloyd Williams ◽  
Nicole J. Rijs
Keyword(s):  
Mass Spectrometry ◽  
Ion Mobility ◽  
Self Assembly ◽  
Functional Materials ◽  
Ion Mobility Mass Spectrometry ◽  
Complex Species ◽  
Structural Characterisation ◽  
Analytical Technique ◽  
Complex Processes ◽  
Analytical Approaches

Nature creates exquisite molecular assemblies, required for the molecular-level functions of life, via self-assembly. Understanding and harnessing these complex processes presents an immense opportunity for the design and fabrication of advanced functional materials. However, the significant industrial potential of self-assembly to fabricate highly functional materials is hampered by a lack of knowledge of critical reaction intermediates, mechanisms, and kinetics. As we move beyond the covalent synthetic regime, into the domain of non-covalent interactions occupied by self-assembly, harnessing and embracing complexity is a must, and non-targeted analyses of dynamic systems are becoming increasingly important. Coordination driven self-assembly is an important subtype of self-assembly that presents several wicked analytical challenges. These challenges are “wicked” due the very complexity desired confounding the analysis of products, intermediates, and pathways, therefore limiting reaction optimisation, tuning, and ultimately, utility. Ion Mobility-Mass Spectrometry solves many of the most challenging analytical problems in separating and analysing the structure of both simple and complex species formed via coordination driven self-assembly. Thus, due to the emerging importance of ion mobility mass spectrometry as an analytical technique tackling complex systems, this review highlights exciting recent applications. These include equilibrium monitoring, structural and dynamic analysis of previously analytically inaccessible complex interlinked structures and the process of self-sorting. The vast and largely untapped potential of ion mobility mass spectrometry to coordination driven self-assembly is yet to be fully realised. Therefore, we also propose where current analytical approaches can be built upon to allow for greater insight into the complexity and structural dynamics involved in self-assembly.

scholarly journals A heterobimetallic tetrahedron from a linear platinum(II)-bis(acetylide) metalloligand

2020 ◽  
Vol 16 ◽  
pp. 2701-2708
Author(s):  
Matthias Hardy ◽  
Marianne Engeser ◽  
Arne Lützen
Keyword(s):  
Mass Spectrometry ◽  
Self Assembly ◽  
Organic Ligand ◽  
Design Concepts ◽  
Assembly Strategy ◽  
Vis Spectroscopy ◽  
Coordination Cages ◽  
Esi Mass Spectrometry

Employing 4-ethynylaniline as a simple organic ligand we were able to prepare the stable trans-bis(acetylide)platinum(II) complex [Pt(L1)2(PBu3)2] as a linear metalloligand. The reaction of this metalloligand with iron(II) cations and pyridine-2-carbaldehyde according to the subcomponent self-assembly approach yielded decanuclear heterobimetallic tetrahedron [Fe4Pt6(L2)12](OTf)8. Thus, combination of these two design concepts – the subcomponent self-assembly strategy and the complex-as-a-ligand approach – ensured a fast and easy synthesis of large heterobimetallic coordination cages of tetrahedral shape with a diameter of more than 3 nm as a mixture of all three possible T-, S 4- and C 3-symmetric diastereomers. The new complexes were characterized by NMR and UV–vis spectroscopy and ESI mass spectrometry. Using GFN2-xTB we generated energy-minimized models of the diastereomers of this cage that further corroborated the results from analytical findings.

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