Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry

The impressive success of mRNA-based vaccines to combat COVID-19 has encouraged biopharmaceutical companies to invest in broader applications of alike vaccines for various diseases. Analytical approaches must keep pace to support this surge in the development of mRNA-based therapies. Intact mass ana...

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Main Authors: Evolène Deslignière, Lauren F. Barnes, Thomas W. Powers, Olga V. Friese, Albert J.R. Heck
Format: Article
Language:English
Published: Elsevier 2025-06-01
Series:Molecular Therapy: Methods & Clinical Development
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Online Access:http://www.sciencedirect.com/science/article/pii/S232905012500049X
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author Evolène Deslignière
Lauren F. Barnes
Thomas W. Powers
Olga V. Friese
Albert J.R. Heck
author_facet Evolène Deslignière
Lauren F. Barnes
Thomas W. Powers
Olga V. Friese
Albert J.R. Heck
author_sort Evolène Deslignière
collection DOAJ
description The impressive success of mRNA-based vaccines to combat COVID-19 has encouraged biopharmaceutical companies to invest in broader applications of alike vaccines for various diseases. Analytical approaches must keep pace to support this surge in the development of mRNA-based therapies. Intact mass analysis of mid- to large mRNA molecules (>1,000 nt) poses significant analytical challenges due to mRNA size, heterogeneity, and instability. Here, we demonstrate how single-particle Orbitrap-based charge detection mass spectrometry (CDMS) and mass photometry (MP) approaches can rapidly measure the mass of various intact high-mass capped mRNAs, up to 9,400 nt (∼3 MDa) in size. While ensemble MS yielded approximate masses for mRNAs <2,000 nt, it failed to provide information on samples of longer sequences. The drawbacks of ensemble MS could be avoided by recording individual ions. Low-charge mRNA components showed unstable ion behavior, hampering initial CDMS measurements, whereas high-charge populations offered better signal-to-noise and reduced charge uncertainty, with drastically improved mass accuracy. Lastly, in-solution MP enabled the measurement of mRNAs with high accuracy, while revealing low amounts of mRNA fragments and dimers that are sometimes overlooked in CDMS. Overall, CDMS and MP provide complementary methods that enable the study of large heterogeneous mRNA without requiring prior digestion or online separation.
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spelling doaj-art-25d5df6171dd404eba510a54a1b6daeb2025-08-20T01:55:11ZengElsevierMolecular Therapy: Methods & Clinical Development2329-05012025-06-0133210145410.1016/j.omtm.2025.101454Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometryEvolène Deslignière0Lauren F. Barnes1Thomas W. Powers2Olga V. Friese3Albert J.R. Heck4Biomolecular Mass Spectrometry and Proteomics, Bijvoet Centre for Biomolecular Research and Utrecht Institute for Pharmaceutical Sciences, University of Utrecht, 3584 CH Utrecht, the Netherlands; Netherlands Proteomics Center, 3584 CH Utrecht, the NetherlandsBioTherapeutics Pharmaceutical Sciences, Pfizer Inc, Chesterfield, MO 63017, USABioTherapeutics Pharmaceutical Sciences, Pfizer Inc, Chesterfield, MO 63017, USABioTherapeutics Pharmaceutical Sciences, Pfizer Inc, Chesterfield, MO 63017, USABiomolecular Mass Spectrometry and Proteomics, Bijvoet Centre for Biomolecular Research and Utrecht Institute for Pharmaceutical Sciences, University of Utrecht, 3584 CH Utrecht, the Netherlands; Netherlands Proteomics Center, 3584 CH Utrecht, the Netherlands; Corresponding author: Albert J.R. Heck, Biomolecular Mass Spectrometry and Proteomics, Bijvoet Centre for Biomolecular Research and Utrecht Institute for Pharmaceutical Sciences, University of Utrecht, 3584 CH Utrecht, the Netherlands.The impressive success of mRNA-based vaccines to combat COVID-19 has encouraged biopharmaceutical companies to invest in broader applications of alike vaccines for various diseases. Analytical approaches must keep pace to support this surge in the development of mRNA-based therapies. Intact mass analysis of mid- to large mRNA molecules (>1,000 nt) poses significant analytical challenges due to mRNA size, heterogeneity, and instability. Here, we demonstrate how single-particle Orbitrap-based charge detection mass spectrometry (CDMS) and mass photometry (MP) approaches can rapidly measure the mass of various intact high-mass capped mRNAs, up to 9,400 nt (∼3 MDa) in size. While ensemble MS yielded approximate masses for mRNAs <2,000 nt, it failed to provide information on samples of longer sequences. The drawbacks of ensemble MS could be avoided by recording individual ions. Low-charge mRNA components showed unstable ion behavior, hampering initial CDMS measurements, whereas high-charge populations offered better signal-to-noise and reduced charge uncertainty, with drastically improved mass accuracy. Lastly, in-solution MP enabled the measurement of mRNAs with high accuracy, while revealing low amounts of mRNA fragments and dimers that are sometimes overlooked in CDMS. Overall, CDMS and MP provide complementary methods that enable the study of large heterogeneous mRNA without requiring prior digestion or online separation.http://www.sciencedirect.com/science/article/pii/S232905012500049XmRNAintact massnative mass spectrometrycharge detection mass spectrometrymass photometrysingle particle
spellingShingle Evolène Deslignière
Lauren F. Barnes
Thomas W. Powers
Olga V. Friese
Albert J.R. Heck
Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry
Molecular Therapy: Methods & Clinical Development
mRNA
intact mass
native mass spectrometry
charge detection mass spectrometry
mass photometry
single particle
title Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry
title_full Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry
title_fullStr Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry
title_full_unstemmed Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry
title_short Characterization of intact mRNA-based therapeutics by charge detection mass spectrometry and mass photometry
title_sort characterization of intact mrna based therapeutics by charge detection mass spectrometry and mass photometry
topic mRNA
intact mass
native mass spectrometry
charge detection mass spectrometry
mass photometry
single particle
url http://www.sciencedirect.com/science/article/pii/S232905012500049X
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