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. 2017 Aug 15;7:8246. doi: 10.1038/s41598-017-08597-4

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© The Author(s) 2017

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

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The analysis of citrullination in human synovial fluid samples. (a) Illustration of protein citrullination by PAD enzyme. (b) Number of detected unique spectra by mass spectrometry in albumin depleted or heparin fractionated synovial fluid samples (n = 11). (c) Correlation of extracellular citrullination (mass spectrometry, MS) and PAD activity (enzyme assay). (d) Detected citrullinated sites of extracellular proteins in synovial fluid samples. (e) The citrullinated extracellular proteins identified in synovial fluids (n = 40). The frequency (%) of samples containing the given citrullinated protein is shown. (f) The relationships of the extracellular citrullinated proteins to selected biological processes according to the GO Database 6/2014 release⁴⁵ appended with current knowledge of the biological role of angiogenin^46–48, MXRA5⁴⁹, PRG4⁵⁰ and EFEMP1⁵¹. IGHM, which is a subunit of IgM is connected to inflammatory response. (g) Citrullination levels of the arginines with a characterized function in individual samples. Only the arginines present in both citrullinated and non-citrullinated peptides were included.