Ion Mobility Mass Spectrometry for Large Synthetic Molecules: Expanding the Analytical Toolbox

Overview

Journal J Am Chem Soc

Publisher American Chemical Society

Specialty Chemistry

Date 2024 Mar 18

PMID 38498971

Authors

Niklas Geue

Richard E P Winpenny

Perdita E Barran

Affiliations

Soon will be listed here.

Abstract

Understanding the composition, structure and stability of larger synthetic molecules is crucial for their design, yet currently the analytical tools commonly used do not always provide this information. In this perspective, we show how ion mobility mass spectrometry (IM-MS), in combination with tandem mass spectrometry, complementary techniques and computational methods, can be used to structurally characterize synthetic molecules, make and predict new complexes, monitor disassembly processes and determine stability. Using IM-MS, we present an experimental and computational framework for the analysis and design of complex molecular architectures such as (metallo)supramolecular cages, nanoclusters, interlocked molecules, rotaxanes, dendrimers, polymers and host-guest complexes.

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References

Miras H, Long D, Kogerler P, Cronin L . Bridging the gap between solution and solid state studies in polyoxometalate chemistry: discovery of a family of [V1M17]-based cages encapsulating two {VVO4} moieties. Dalton Trans. 2007; (2):214-21. DOI: 10.1039/b714285d. View

Lloyd Williams O, Rusli O, Ezzedinloo L, Dodgen T, Clegg J, Rijs N . Automated Structural Activity Screening of β-Diketonate Assemblies with High-Throughput Ion Mobility-Mass Spectrometry. Angew Chem Int Ed Engl. 2023; 63(4):e202313892. DOI: 10.1002/anie.202313892. View

Gu L, Wu F, Yang S, Xu F, Dai X, Jiang Y . Direct distinction of ibuprofen and flurbiprofen enantiomers by ion mobility mass spectrometry of their ternary complexes with metal cations and cyclodextrins in the gas phase. J Sep Sci. 2021; 44(12):2474-2482. DOI: 10.1002/jssc.202100025. View

Bennett T, Geue N, Timco G, Whitehead G, Vitorica-Yrezabal I, Barran P . Studying Cation Exchange in {CrCo} Pseudorotaxanes: Preparatory Studies for Making Hybrid Molecular Machines. Chemistry. 2024; 30(37):e202400432. PMC: 11497308. DOI: 10.1002/chem.202400432. View

Wang J, Wolf R, Caldwell J, Kollman P, Case D . Development and testing of a general amber force field. J Comput Chem. 2004; 25(9):1157-74. DOI: 10.1002/jcc.20035. View

Rauschenbach S, Ternes M, Harnau L, Kern K . Mass Spectrometry as a Preparative Tool for the Surface Science of Large Molecules. Annu Rev Anal Chem (Palo Alto Calif). 2016; 9(1):473-98. DOI: 10.1146/annurev-anchem-071015-041633. View

Dixit S, Polasky D, Ruotolo B . Collision induced unfolding of isolated proteins in the gas phase: past, present, and future. Curr Opin Chem Biol. 2017; 42:93-100. PMC: 5828980. DOI: 10.1016/j.cbpa.2017.11.010. View

May J, Russell D . A mass-selective variable-temperature drift tube ion mobility-mass spectrometer for temperature dependent ion mobility studies. J Am Soc Mass Spectrom. 2011; 22(7):1134-45. DOI: 10.1007/s13361-011-0148-2. View

Mathieson J, Cooper G, Pickering A, Keller M, Long D, Newton G . Monitoring the formation of coordination complexes using electrospray mass spectrometry. Chem Asian J. 2009; 4(5):681-7. DOI: 10.1002/asia.200900007. View

10.

Rainey M, Watson C, Asef C, Foster M, Baker E, Fernandez F . CCS Predictor 2.0: An Open-Source Jupyter Notebook Tool for Filtering Out False Positives in Metabolomics. Anal Chem. 2022; 94(50):17456-17466. PMC: 9772062. DOI: 10.1021/acs.analchem.2c03491. View

11.

Erbas-Cakmak S, Leigh D, McTernan C, Nussbaumer A . Artificial Molecular Machines. Chem Rev. 2015; 115(18):10081-206. PMC: 4585175. DOI: 10.1021/acs.chemrev.5b00146. View

12.

Schultz A, Li X, Barkakaty B, Moorefield C, Wesdemiotis C, Newkome G . Stoichiometric self-assembly of isomeric, shape-persistent, supramacromolecular bowtie and butterfly structures. J Am Chem Soc. 2012; 134(18):7672-5. DOI: 10.1021/ja303177v. View

13.

Schulte T, Holstein J, Clever G . Chiral Self-Discrimination and Guest Recognition in Helicene-Based Coordination Cages. Angew Chem Int Ed Engl. 2019; 58(17):5562-5566. PMC: 6563462. DOI: 10.1002/anie.201812926. View

14.

Saintmont F, De Winter J, Chirot F, Halin E, Dugourd P, Brocorens P . How Spherical Are Gaseous Low Charged Dendrimer Ions: A Molecular Dynamics/Ion Mobility Study?. J Am Soc Mass Spectrom. 2020; . DOI: 10.1021/jasms.0c00113. View

15.

Norgate E, Upton R, Hansen K, Bellina B, Brookes C, Politis A . Cold Denaturation of Proteins in the Absence of Solvent: Implications for Protein Storage. Angew Chem Int Ed Engl. 2022; 61(25):e202115047. PMC: 9325448. DOI: 10.1002/anie.202115047. View

16.

Crotty S, Gerislioglu S, Endres K, Wesdemiotis C, Schubert U . Polymer architectures via mass spectrometry and hyphenated techniques: A review. Anal Chim Acta. 2016; 932:1-21. DOI: 10.1016/j.aca.2016.05.024. View

17.

Zhang X, Srot V, Wu X, Kern K, van Aken P, Anggara K . Controlled Formation of Nanoribbons and Their Heterostructures via Assembly of Mass-Selected Inorganic Ions. Adv Mater. 2024; 36(23):e2310817. DOI: 10.1002/adma.202310817. View

18.

Wang H, Zhou L, Zheng Y, Wang K, Song B, Yan X . Double-Layered Supramolecular Prisms Self-Assembled by Geometrically Non-equivalent Tetratopic Subunits. Angew Chem Int Ed Engl. 2020; 60(3):1298-1305. DOI: 10.1002/anie.202010805. View

19.

Scarff C, Snelling J, Knust M, Wilkins C, Scrivens J . New structural insights into mechanically interlocked polymers revealed by ion mobility mass spectrometry. J Am Chem Soc. 2012; 134(22):9193-8. DOI: 10.1021/ja2118656. View

20.

Gabelica V, Shvartsburg A, Afonso C, Barran P, Benesch J, Bleiholder C . Recommendations for reporting ion mobility Mass Spectrometry measurements. Mass Spectrom Rev. 2019; 38(3):291-320. PMC: 6618043. DOI: 10.1002/mas.21585. View