Probing the structure of giant fullerenes by high resolution trapped ion mobility spectrometry

Weis, Patrick; Hennrich, Frank; Fischer, Robert F. H.; Schneider, Erik; Neumaier, Marco; Kappes, Manfred M.

doi:10.1039/c9cp03326b

Cited by 15 publications

(23 citation statements)

References 66 publications

(144 reference statements)

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“…It relies on determination of the drift time of an ion in an inert collision gas (typically helium or nitrogen) guided by an electrical field. With the recent development of several instrumental variants which can provide greatly improved IMS resolution, the method has gained in importance, for example, in studies of proteins, [25] polysaccharides, [26] and fullerenes, [27] and can now provide an additional useful identification parameter in proteomics [28] . In our measurements, we used a high‐resolution variant of IMS, trapped ion mobility spectrometry (TIMS) coupled with a ToF‐mass spectrometer (timsTOF™, Bruker).…”

Section: Resultsmentioning

confidence: 99%

A Synthetic Strategy for Cofacial Porphyrin‐Based Homo‐ and Heterobimetallic Complexes

Schissler

Schneider

Felker

et al. 2021

Chemistry A European J

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We present a straightforward and generally applicable synthesis route for cofacially linked homo‐ and heterobimetallic porphyrin complexes. The protocol allows the synthesis of unsymmetrical aryl‐based meso‐meso as well as β‐meso‐linked porphyrins. Our method significantly increases the overall yield for the published compound known as o‐phenylene‐bisporphyrin (OBBP) by a factor of 6.8. Besides the synthesis of 16 novel homobimetallic complexes containing MnIII, FeIII, NiII, CuII, ZnII, and PdII, we achieved the first single‐crystal X‐ray structure of an unsymmetrical cofacial benzene‐linked porphyrin dimer containing both planar‐chiral enantiomers of a NiII2 complex. Additionally, this new methodology allows access to heterobimetallic complexes such as the FeIII‐NiII containing carbon monoxide dehydrogenase active site analogue. The isolated species were investigated by various techniques, including ion mobility spectrometry, DFT calculations, and UV/Vis spectroscopy. This allowed us to probe the influence of interplane distance on Soret band splitting.

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Section: Resultsmentioning

confidence: 99%

A Synthetic Strategy for Cofacial Porphyrin‐Based Homo‐ and Heterobimetallic Complexes

Schissler

Schneider

Felker

et al. 2021

Chemistry A European J

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“…Additionally, Viehland accounts for anisotropic effects on the mobility of atomic spherical ions, ultimately concluding that computational methods do not match the experimental data and theoreticians should strive to develop a method to extract inelastic collision information out of experimental mobility data . It seems this is still an existing problem for the IMS community since Weis et al end up adjusting polarizability and anisotropy as variables in their computations to make their computational cross sections for fullerenes match their experimental cross sections measured in their TIMS …”

Section: Resultsmentioning

confidence: 99%

“…While accounting for anisotropic collision might enhance the rigor associated with the ion–neutral interaction, the impact of this parameter is largely unknown and extremely difficult to quantitatively assess experimentally with the ions and neutral often probed currently within the field . Nevertheless, as the core understanding of the factors contributing to the observed mobility improve, this parameter requires considerations.…”

Section: Resultsmentioning

confidence: 99%

“…48 It seems this is still an existing problem for the IMS community since Weis et al end up adjusting polarizability and anisotropy as variables in their computations to make their computational cross sections for fullerenes match their experimental cross sections measured in their TIMS. 49 While accounting for anisotropic collision might enhance the rigor associated with the ion−neutral interaction, the impact of this parameter is largely unknown and extremely difficult to quantitatively assess experimentally with the ions and neutral often probed currently within the field. 49 Nevertheless, as the core understanding of the factors contributing to the observed mobility improve, this parameter requires considerations.…”

Section: T H I S C O N T E N T Imentioning

confidence: 99%

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Assessing the Impact of Drift Gas Polarizability in Polyatomic Ion Mobility Experiments

2020

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Due to the core assumptions of kinetic theory and the drive toward realizing reproducible gas-phase measurements, ion mobility experiments are commonly conducted in the presence of an inert, neat buffer gas, usually nitrogen or helium. Mixing drift gases in defined, static ratios can provide useful information not only for optimizing the separation of analytes but also for defining the interaction between the ion and neutral particle. In a foundational effort, we seek to validate the role of the drift gas polarizability on the observed mobility of the ions by systematically mixing drift gases to discretely access a range of bulk gas polarizabilities not given by pure drift gases. Compared to historical efforts to probe the role of polarizability on the ion−neutral collisional cross section where a linear relationship was assumed, the data collected in the present effort clearly illustrate a quadratic dependency of the ion−neutral particle collision cross section and polarizability (R 2 > 0.999). When translating these data into the mobility dimension, we illustrate that the gas-phase mobility of polyatomic ions conforms to Blanc's law. These observations combined with considerations related to Langevin's polarization limit provide an experimental mechanism to estimate to what degree an ion−neutral interaction conforms to either the hard-sphere or induced-dipole model. To support these observations, additional comparisons are made with the respective reduced masses, polarizabilities, and mobilities of ions in mixtures where different degrees of hard-sphere interactions are present.

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“…Presently therefore, the power of high resolution ESI‐(MS)‐IMS‐MS lies not so much in the “inverse determination” of the exact gas‐phase molecular ion structures, instead it is more useful for distinguishing (and separating) the different isomeric shapes present after electrospraying. [24] In this context it is important to realize, that the barriers to conformer interconversion are typically much larger in gas‐phase than in solution. Thus ESI‐IMS can potentially serve to “freeze out” parts of the conformer space which would otherwise be too rapidly sampled by solvated molecules in room temperature solutions.…”

Section: Introductionmentioning

confidence: 99%

Advancing Inorganic Coordination Chemistry by Spectroscopy of Isolated Molecules: Methods and Applications

Niedner‐Schatteburg

Kappes

2021

Chemistry A European J

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A unique feature of the work carried out in the Collaborative Research Center 3MET continues to be its emphasis on innovative, advanced experimental methods which hyphenate mass-selection with further analytical tools such as laser spectroscopy for the study of isolated molecular ions. This allows to probe the intrinsic properties of the species of interest free of perturbing solvent or matrix effects. This review explains these methods and uses examples from past and ongoing 3MET studies of specific classes of multicenter metal complexes to illustrate how coordination chemistry can be advanced by applying them. As a corollary, we will show how the challenges involved in providing welldefined, for example monoisomeric, samples of the molecular ions have helped to further improve the methods themselves thus also making them applicable to many other areas of chemistry.

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Probing the structure of giant fullerenes by high resolution trapped ion mobility spectrometry

Abstract: We present high-resolution trapped ion mobility spectrometry (TIMS) measurements for fullerene ions in molecular nitrogen.

Cited by 15 publications

References 66 publications

A Synthetic Strategy for Cofacial Porphyrin‐Based Homo‐ and Heterobimetallic Complexes

A Synthetic Strategy for Cofacial Porphyrin‐Based Homo‐ and Heterobimetallic Complexes

Assessing the Impact of Drift Gas Polarizability in Polyatomic Ion Mobility Experiments

Advancing Inorganic Coordination Chemistry by Spectroscopy of Isolated Molecules: Methods and Applications

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