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A novel LC–MS method using collagen marker peptides for species identification of glue applicable to samples with multiple animal origins

Yuki Kumazawa · Yuki Taga · Miho Takashima · Shunji Hattori

27 citations0/0 files storedHeritage Science

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Cultural Heritage Materials Analysis Collagen: Extraction and Characterization Identification and Quantification in Food

Abstract

Abstract Animal glues derived from collagen-rich tissue are widely used as adhesives and binders in artworks. Identification of the animal source of glue is important not only to understand the artistic technique and historical background, but also to conduct appropriate treatment for restoration and conservation of artworks. Recently, mass spectrometric approaches have been used for species identification of glue. However, it appears that the existing methods were not applied to samples containing multiple animal sources, and the range of target species has been limited because of incomplete sequence information of collagen in public databases. In the present study, we established a novel method for discrimination of glues from eight animals applicable to samples with multiple animal origins. Trypsin-digested glue samples were analyzed by LC–MS in multiple reaction monitoring mode, and the animal source was determined based on the detection patterns of 12 type I collagen-derived marker peptides. Using the database-independent method, we successfully identified the animal source of commercial products and found the declared species for some glues to be incorrect. In addition, some products were identified to contain two different animal origins. Relative abundance of the animal origins in several impure glues was estimated using the marker peptides, which helped to speculate the reason for the detection of multiple species. We analyzed a painting (The Harvest by Camille Pissarro, 1882) and clarified that glues used in the ground and size layers of the canvas were derived from cattle (~ 65%) and sheep (~ 35%).

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References

2007Animal glues: a review of their key properties relevant to conservation 2011Deamidation at Asparagine and Glutamine As a Major Modification upon Deterioration/Aging of Proteinaceous Binders in Mural Paintings 2010Immunodetection of Proteins in Ancient Paint Media 2011Identification of Animal Glue Species in Artworks Using Proteomics: Application to a 18th Century Gilt Sample 2009Tryptic peptide analysis of protein binders in works of art by liquid chromatography–tandem mass spectrometry 2005Analysis of organic colouring and binding components in colour layer of art works 2013Identification of protein binders in artworks by MALDI-TOF/TOF tandem mass spectrometry 2006An evaluation of GC‐MS and HPLC‐FD methods for analysis of protein binders in paintings

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2020In Situ Hydrogel Extraction with Dual-Enzyme Digestion of Proteinaceous Binders: the Key for Reliable Mass Spectrometry Investigations of Artworks 2021A comparative study on the extraction effects of common agents on collagen-based binders in mural paintings 2018Characterization of proteins in cultural heritage using MALDI–TOF and LC–MS/MS mass spectrometric techniques 2022Paleoproteomic profiling for identification of animal skin species in ancient Egyptian archaeological leather using liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS)

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