Dynamic Motion in Crown Ether Dendrimer Complexes: A “Spacewalk” on the Molecular Scale

Winkler, Henrik D. F.; Weimann, Dominik P.; Springer, Andreas; Schalley, Christoph A.

doi:10.1002/anie.200902437

Cited by 30 publications

(17 citation statements)

References 28 publications

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“…(3) The CE is not permanently bound to one specific site, but can "walk" between them when they are close enough to each other. This phenomenon was reported earlier 30,31 and might offer an explanation for the increase in the effective binding strength of the wt. Next, the 3CE complex of each variant was isolated, fragmented and its depletion plotted as described above (Fig.…”

Section: Energy-resolved Collision Induced Dissociation Experimentssupporting

confidence: 82%

Gas-phase microsolvation of ubiquitin: investigation of crown ether complexation sites using ion mobility-mass spectrometry

Göth

Lermyte

Schmitt

et al. 2016

Analyst

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In this study the gas-phase structure of ubiquitin and its lysine-to-arginine mutants was investigated using ion mobility-mass spectrometry (IM-MS) and electron transfer dissociation-mass spectrometry (ETD-MS). Crown ether molecules were attached to positive charge sites of the proteins and the resulting noncovalent complexes were analysed. Collision induced dissociation (CID) experiments revealed relative energy differences between the wild type and the mutant crown-ether complexes. ETD-MS experiments were performed to identify the crown ether binding sites. Although not all of the binding sites could be revealed, the data confirm that the first crown ether is able to bind to the N-terminus. IM-MS experiments show a more compact structure for specific charge states of wild type ubiquitin when crown ethers are attached. However, data on ubiquitin mutants reveal that only specific lysine residues contribute to the effect of charge microsolvation. A compaction is only observed for one of the investigated mutants, in which the lysine has no proximate interaction partner. On the other hand when the lysine residues are involved in salt bridges, attachment of crown ethers has little effect on the structure.

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Section: Energy-resolved Collision Induced Dissociation Experimentssupporting

confidence: 82%

Gas-phase microsolvation of ubiquitin: investigation of crown ether complexation sites using ion mobility-mass spectrometry

Göth

Lermyte

Schmitt

et al. 2016

Analyst

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“…Does monovalent BC7 “walk” along the periphery of POPAM dendrimers from one side chain to another? In an earlier study7b on monovalent crown ether–POPAM complexes, HDX reactions were used to demonstrate that [18]crown‐6 migrates directly together with a proton from an ammonium group to an amine side chain. The next step in the present work is thus to evaluate whether BC7 behaves analogously.…”

Section: Resultsmentioning

confidence: 99%

Multivalency in the Gas Phase: H/D Exchange Reactions Unravel the Dynamic “Rock ’n’ Roll” Motion in Dendrimer–Dendrimer Complexes

Schlaich

Schalley

2013

Chemistry A European J

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Noncovalent dendrimer–dendrimer complexes were successfully ionized by electrospray ionization of partly protonated amino‐terminated polypropylene amine (POPAM) and POPAM dendrimers fully functionalized with benzo[21]crown‐7 on all branches. Hydrogen/deuterium exchange (HDX) experiments conducted on dendrimer–dendrimer complexes in the high vacuum of a mass spectrometer give rise to a complete exchange of all labile NH hydrogen atoms. As crown ethers represent noncovalent protective groups against HDX reactions on the ammonium group to which they are coordinated, this result provides evidence for a very dynamic binding situation: each crown is mobile enough to move from one ammonium binding site to another. Schematically, one might compare this motion with two rock ’n’ roll dancers that swirl around each other without completely losing all contact at any time. Although the multivalent attachment certainly increases the overall affinity, the “microdynamics” of individual site binding and dissociation remains fast.

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“…The latter structure is similar to the one found for GlyHisNa + by MP2 calculations by Kapota and Ohanessian. [29] However, in the carnosine case the β-alanyl side chain allows for more flexibility so that the His-N binding is replaced by the H 2 N group and the structures CarX + (I) result as the minimum structures. In the common nomenclature these structures are considered as charge solvated (CS).…”

Section: Discussionmentioning

confidence: 99%

“…The coordination of histidine to alkali [26] and alkaline earth metal ions [27] and the structure of protonated histidine [28] have been studied recently by calculations, IRMPD spectroscopy and H/D exchange (HDX) measurements, respectively. HDX is also a useful technique for the study of supramolecular adduct-peptide structures [29].…”

Section: Introductionmentioning

confidence: 99%

The Interaction of the Dipeptide Carnosine With Alkali Metal Ions Studied by Ion Trap Mass Spectrometry

Menges

Riehn

Niedner‐Schatteburg³

2011

Zeitschrift Für Physikalische Chemie

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The complexation of alkali metal ions and the proton X + (X = H, Li, Na, K, Rb, Cs) by β-alanyl-L-histidine (carnosine, Car) was investigated by electrospray ionization mass spectrometry (ESI-MS) and MS/MS fragmentation studies. Collision-induced dissociation (CID) breakdown curves were recorded and the resulting apparent activation energies were compared to DFT calculations of binding energies at the B3LYP/cc-pVDZ level of theory. Additionally, the influence of metal complexation on hydrogen/deuterium exchange of CarX + with D 2 O was tested. Our investigations characterize the structures of Car-alkali complexes and elucidate the interaction with the differently sized solvated metal cations.

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Dynamic Motion in Crown Ether Dendrimer Complexes: A “Spacewalk” on the Molecular Scale

Cited by 30 publications

References 28 publications

Gas-phase microsolvation of ubiquitin: investigation of crown ether complexation sites using ion mobility-mass spectrometry

Gas-phase microsolvation of ubiquitin: investigation of crown ether complexation sites using ion mobility-mass spectrometry

Multivalency in the Gas Phase: H/D Exchange Reactions Unravel the Dynamic “Rock ’n’ Roll” Motion in Dendrimer–Dendrimer Complexes

The Interaction of the Dipeptide Carnosine With Alkali Metal Ions Studied by Ion Trap Mass Spectrometry

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