Proteoform‐Selective Imaging of Tissues Using Mass Spectrometry**
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Abstract
Unraveling the complexity of biological systems relies on the development of new approaches for spatially resolved proteoform‐specific analysis of the proteome. Herein, we employ nanospray desorption electrospray ionization mass spectrometry imaging (nano‐DESI MSI) for the proteoform‐selective imaging of biological tissues. Nano‐DESI generates multiply charged protein ions, which is advantageous for their structural characterization using tandem mass spectrometry (MS/MS) directly on the tissue. Proof‐of‐concept experiments demonstrate that nano‐DESI MSI combined with on‐tissue top‐down proteomics is ideally suited for the proteoform‐selective imaging of tissue sections. Using rat brain tissue as a model system, we provide the first evidence of differential proteoform expression in different regions of the brain.
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Cites
How many human proteoforms are there?
Aebersold, R., Agar, J. N., Amster, I. J., Baker, M. S., Bertozzi, C. R., Boja, E. S., Costello, C. E., Cravatt, B. F., Fenselau, C., Garcia, B. A., et al. (2018) · Nature Chemical Biology · doi:10.1038/nchembio.2576 · Cited by 907 · see citing works
Self-citationZhu, Y., Piehowski, P. D., Zhao, R., Chen, J., Shen, Y., Moore, R. J., Shukla, A. K., Petyuk, V. A., Campbell-Thompson, M., Mathews, C. E., et al. (2018) · Nature Communications · doi:10.1038/s41467-018-03367-w · Cited by 587 · see citing works
Decoding protein modifications using top-down mass spectrometry
Siuti, N., & Kelleher, N. L. (2007) · Nature Methods · doi:10.1038/nmeth1097 · Cited by 503 · see citing works
Self-citationThe Human Proteoform Project: Defining the human proteome
Smith, L. M., Agar, J. N., Chamot-Rooke, J., Danis, P. O., Ge, Y., Loo, J. A., Paša-Tolić, L., Tsybin, Y. O., Kelleher, N. L., & The Consortium for Top-Down Proteomics (2021) · Science Advances · doi:10.1126/sciadv.abk0734 · Cited by 242 · see citing works
Self-citationLermyte, F., Tsybin, Y. O., O’Connor, P. B., & Loo, J. A. (2019) · Journal of the American Society for Mass Spectrometry · doi:10.1007/s13361-019-02201-x · Cited by 132 · see citing works
Zhou, M., Uwugiaren, N., Williams, S. M., Moore, R. J., Zhao, R., Goodlett, D., Dapic, I., Paša-Tolić, L., & Zhu, Y. (2020) · Analytical Chemistry · doi:10.1021/acs.analchem.0c00467 · Cited by 62 · see citing works
Riley, N. M., Sikora, J. W., Seckler, H. S., Greer, J. B., Fellers, R. T., LeDuc, R. D., Westphall, M. S., Thomas, P. M., Kelleher, N. L., & Coon, J. J. (2018) · Analytical Chemistry · doi:10.1021/acs.analchem.8b01638 · Cited by 43 · see citing works
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- Authors
- Yang, M., Hu, H., Su, P., Thomas, P. M., Camarillo, J. M., Greer, J. B., Early, B. P., Fellers, R. T., Kelleher, N. L., & Laskin, J.
- Affiliations
- Purdue University West Lafayette (US)
- Northwestern University (US)
- Corresponding author
- Kelleher, Neil L.
- Laskin, Julia
- ORCID
- Venue
- Angewandte Chemie International Edition
- Publisher
- Wiley
- Published
- 2022-05-17
- Volume
- 61
- Issue
- 29
- Pages
- e202200721-e202200721
- ISSN
- 1433-7851 (ISSN-L)
- 1521-3773
- PMC
- PMC9276647
- OpenAlex
- W4225257233
- Cited by
- 54
- References
- 7
- Citations by year
- 2026: 6 · 2025: 16 · 2024: 12 · 2023: 14 · 2022: 6
- FWCI
- 4.33
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- Angewandte Chemie International Edition (publishedVersion, cc-by-nc)
- ChemRxiv (acceptedVersion, cc-by-nc)
- PubMed Central (publishedVersion, cc-by-nc)
- PubMed (publishedVersion)
- Funders
- Office of Strategic Coordination (UG3HL145593, UH3CA255132, UH3CA246635, P41GM108569)
- National Science Foundation (NSF-1916691, NSF-1808136, NSF-2108729)
- Topics
- Physical Sciences › Chemistry › Spectroscopy › Mass Spectrometry Techniques and Applications
- Physical Sciences › Chemistry › Spectroscopy › Advanced Proteomics Techniques and Applications
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Metabolomics and Mass Spectrometry Studies
- Keywords
- top-down proteomics, spatial proteomics, tissue sections, rat brain, tandem mass spectrometry
- MeSH terms
- Animals, Ions, Proteome, Spectrometry, Mass, Electrospray Ionization, Proteomics, Rats, Tandem Mass Spectrometry
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