Native mass spectrometry (MS) is usually conducted in the positive-ion mode; however, in some cases, it is advantageous to use the negative-ion polarity. Challenges associated with native MS using ensemble measurements (i.e., the measurement of many ions at a time as opposed to the measurement of the charge and the mass-to-charge ratio of individual ions) include narrow charge state distributions with the potential for an overlap in neighboring charge states. These issues can either compromise or preclude confident charge state (and hence mass) determination. Charge state determination in challenging instances can be enabled via the attachment of multiply charged ions of opposite polarity. Multiply charged ion attachment facilitates the resolution of charge states and generates mass-to-charge (/) information across a broad / range. In this work, we demonstrated the attachment of multiply charged cations to anionic complexes generated under native MS conditions. To illustrate the flexibility available in selecting the mass and charge of the reagents, the 15+ and 20+ charge states of horse skeletal muscle apomyoglobin and the 20+ and 30+ charge states of bovine carbonic anhydrase were demonstrated to attach to model complex anions derived from either β-galactosidase or GroEL. The exclusive attachment of reagent ions is observed with no evidence for proton transfer, which is the key for the unambiguous interpretation of the post-ion/ion reaction product ion spectrum. To illustrate the application to mixtures of complex ions, the 10+ charge state of bovine ubiquitin was attached to mixtures of anions generated from the 30S and 50S particles of the ribosome. Six and five major components were revealed, respectively. In the case of the 50S anion population, it was shown that the attachment of two 30+ cations of carbonic anhydrase revealed the same information as the attachment of six 10+ cations of ubiquitin. In neither case was the intact 50S particle observed. Rather, particles with different combinations of missing components were observed. This work demonstrated the utility of multiply charged cation attachment to facilitate charge state assignments in native MS ensemble measurements of heterogeneous mixtures.
Download full-text PDF |
Source |
---|---|
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9670251 | PMC |
http://dx.doi.org/10.1021/acs.analchem.1c04875 | DOI Listing |
Se Pu
January 2025
West China School of Pharmacy, Sichuan University, Chengdu 610041, China.
Ambient mass spectrometry imaging (MSI) enables hundreds of analytes in tissue sections to be directly mapped at atmospheric pressure with minimal sample preparation. This field is currently experiencing rapid growth, with numerous reported ambient ionization techniques resulting in a "hundred flowers bloom" situation. Nanospray desorption electrospray ionization (nano-DESI), developed by the Laskin group in 2010, is a widely used liquid-extraction-based ambient ionization technique that was first used for mass spectrometry imaging of tissue in 2012.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Departament FQA, Facultat de Física, Universitat de Barcelona, Av. Diagonal 645, 08028 Barcelona, Spain.
We study superfluid helium droplets multiply charged with Na+ or Ca+ ions. When stable, the charges are found to reside in equilibrium close to the droplet surface, thus representing a physical realization of Thomson's model. We find the minimum radius of the helium droplet that can host a given number of ions using a model whose physical ingredients are the solvation energy of the cations, calculated within the helium density functional theory approach, and their mutual Coulomb repulsion energy.
View Article and Find Full Text PDFLangmuir
December 2024
College of Textile Science and Engineering, Zhejiang Sci-Tech University, Hangzhou 310018, China.
Perovskite films often suffer from surface and grain boundary defects, including uncoordinated ions, lattice distortions, and dangling bonds, coupled with lattice distortions due to solvent volatilization anisotropy and the thermal expansion coefficient. Such defects severely compromise both the photovoltaic efficiency and long-term solar cell stability. Here, fluorinated polyurethane (FPU) was synthesized and introduced into the perovskite precursor as a multifunctional additive.
View Article and Find Full Text PDFElectrophoresis
November 2024
Institute of Organic Chemistry and Biochemistry of the Czech Academy of Sciences, Prague, Czech Republic.
J Phys Chem A
November 2024
Laboratoire de Chimie et Physique Quantiques, Université Toulouse III─Paul Sabatier, Toulouse 31062, France.
In quantum chemistry, single-reference Coupled Cluster theory, and its refinements introduced by Bartlett, has become a "gold-standard" predictive method for taking into account electronic correlations in molecules. In this article, we introduce a new formalism based on a Coupled Cluster expansion of the wave function that is suited to describe model periodic systems and apply this methodology to the case of hole-doped antiferromagnetic two-dimensional (2D)-square spin-lattices as a proof of concept. More precisely, we focus our study on 1/5 and 1/7 doping ratios and discuss the possible ordering effect due to large hole-hole repulsion.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!