Stepwise reduction of interlocked viologen-based complexes in the gas phase

Marshall, David L.; Poad, Berwyck L. J.; Luis, Ena T.; Rodrigues, Rafael Da Silva; Blanksby, Stephen J.; Mullen, Kathleen M.

doi:10.1039/d0cc05115b

Cited by 5 publications

(3 citation statements)

References 32 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Interestingly, M III containing oligomers did not exhibit the same pattern, as the sulfonic groups of the porphyrins could readily bind to the central metals. It could be interesting to reduce or oxidise the metal centre incorporated in the metalloporphyrin and to observe the potential structural transformation by IMS-MS (Marshall et al, 2020).…”

Section: Structural Identificationmentioning

confidence: 99%

“…It was found that for M II containing oligomers, the charge state of the oligomer, and the corresponding number of sodium counterions, dictated if the structure formed would be “open” or “closed.” Interestingly, M III containing oligomers did not exhibit the same pattern, as the sulfonic groups of the porphyrins could readily bind to the central metals. It could be interesting to reduce or oxidise the metal centre incorporated in the metalloporphyrin and to observe the potential structural transformation by IMS-MS ( Marshall et al, 2020 ).…”

Section: Applications Of Ion Mobility Mass Spectrometry To Study Coordination Driven Self-assemblymentioning

confidence: 99%

See 1 more Smart Citation

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

Williams

Rijs

2021

Front. Chem.

View full text Add to dashboard Cite

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.

show abstract

Section: Structural Identificationmentioning

confidence: 99%

Section: Applications Of Ion Mobility Mass Spectrometry To Study Coordination Driven Self-assemblymentioning

confidence: 99%

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

Williams

Rijs

2021

Front. Chem.

View full text Add to dashboard Cite

show abstract

“…Thepresent study exploits the option of electron-transfer dissociation (ETD) [28] offered by mass spectrometry (MS) platforms to selectively generate and isolate intermediate oxidation states.W hile ETD has been previously used to characterize supramolecular complexes, [29][30][31][32] we aim here to benefit from the energy-tempering properties of the buffer gas as aw ay to perform electron transfers without dissociation [33,34] and induce successive charge reductions of viologen motifs [35] embedded within [4]5NPR. Theg as-phase equilibrium geometries of the consecutive products are subsequently interrogated structurally using MS interfaced with complementary structure-sensitive techniques,that is,ion mobility [36] (IM) and infrared ion spectroscopy [37] (IRIS).…”

Section: Introductionmentioning

confidence: 99%

Radical‐Pairing Interactions in a Molecular Switch Evidenced by Ion Mobility Spectrometry and Infrared Ion Spectroscopy

et al. 2021

View full text Add to dashboard Cite

The digital revolution sets am ilestone in the progressive miniaturization of working devices and in the underlying advent of molecular machines.F oldamers involving mechanically entangled components with modular secondary structures are among the most promising designs for molecular switch-based applications.Characterizing the nature and dynamics of their intramolecular network following the application of astimulus is the key to their performance.Here, we use non-dissociative electron transfer as ar eductive stimulus in the gas phase and probe the consecutive co-conformational transitions of ad onor-acceptor oligorotaxane foldamer using electrospraym ass spectrometry interfaced with ion mobility and infrared ion spectroscopy. Ac omparison of collision cross section distributions for analogous closed-shell and radical molecular ions sheds light on their respective formation energetics,while variations in their respective infrared absorption bands evidence changes in intramolecular organization as the foldamer becomes more compact. These differences are compatible with the advent of radical-pairing interactions.

show abstract

Radical‐Pairing Interactions in a Molecular Switch Evidenced by Ion Mobility Spectrometry and Infrared Ion Spectroscopy

Hanozin

Mignolet

Martens³

et al. 2021

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Stepwise reduction of interlocked viologen-based complexes in the gas phase

Abstract: Thinking outside the (blue)box: electron transfer mass spectrometry as a dual-purpose synthetic and analytical tool for supramolecular complexes.

Cited by 5 publications

References 32 publications

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

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

Radical‐Pairing Interactions in a Molecular Switch Evidenced by Ion Mobility Spectrometry and Infrared Ion Spectroscopy

Radical‐Pairing Interactions in a Molecular Switch Evidenced by Ion Mobility Spectrometry and Infrared Ion Spectroscopy

Contact Info

Product

Resources

About