Evaluation of the deteriorating effects of microbial primary metabolites on silk fibres.

The silk biodegradation process remains unclear and requires elucidation with advanced analytical tools. To address this challenge, the role of microbial primary metabolites in the deterioration of ancient silk was investigated using metabolomics and proteomics techniques in this work. The oxalic and palmitic acids were separately identified as the most abundant organic and fatty acid metabolites for silk-fabric deterioration via metabolomics. Proteomics showed that oxalic acid accelerated the degradation of silk proteins, revealing changes at the molecular level in silk. A high concentration of oxalic acid promoted the dissolution of peptides by activating the cleavage activity of various amino acids on the molecular chain of silk protein. Palmitic acid formed sedimentary particulate matter with peptides solubilised from silk proteins, indicating the possibility that traces of ancient-silk proteins remained in the fatty acids. The work presented new techniques and concepts for studying the degradation of historical fabrics and contributed to the proposal of effective measures to prevent microbial attack on silk.

Microbial degradation mechanism of historical silk revealed by proteomics and metabolomics.

Archaeological silk undergoes destructive and irreversible changes during the natural process of decay. However, in-depth studies on the influence of this biological factor are still lacking. Here, a combination of proteomics and metabolomics is proposed for the first time to explore the interaction between bacteria and historical silk during biodegradation, which provides information on changes at the molecular level of proteins and bacterial metabolites. Morphological observation revealed biofilms produced by Stenotrophomonas maltophilia and Pseudomonas alcaligenes when cultured in the stationary phase and confirmed severe deterioration of silk. Proteomics showed that S. maltophilia had an unbiased effect on silk fibroin, indicating its ability to disrupt both heavy and light chains, as well as other proteins, while P. alcaligenes showed an affinity for more disordered proteins. Analysis of bacterial metabolites showed that overall activity reduction and significant accumulation of fatty acid and phenol metabolites occurred after silk addition, suggesting that the presence of silk may inhibit the activity of an individual strain. This study provides a new insight into the microbial degradation mechanism of archaeological silk.

Molecular Evidence of Structural Changes in Silk Using Unlimited Degradation Mass Spectrometry.

Proteomics has important uses in archeological science because it can distinguish species, reveal the evolution of paleontology, and provide biological evidence of historical events. However, this technique still has full potential in the study of silk aging mechanisms. In this work, we propose a strategy combining unlimited degradation with mass-spectrometry-based proteomics techniques, which interpret protein fragmentation propensity and secondary structure changes by detecting content changes of specific peptide groups in complex proteomes. This approach was employed to study the conformational changes in silk microscopic crystals after heat treatment. Combining conventional mechanics and crystallographic characterization, a thermal aging degradation mechanism model was proposed. At the same time, it explained the interesting problem that the crystallinity remained unchanged, but the mechanical properties decreased significantly. Focusing on the unlimited degradation process, this method will be widely applicable to the study of silk and wool aging processes and regenerated silk fibroin.