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评估用于先进材料的寡肽修饰聚合物长丝的标签稳定性:紫外线暴露和生物降解研究。

Assessing Label Stability in Oligopeptide-Modified Polymer Filament for Advanced Materials: Ultraviolet Exposure and Biodegradation Study.

作者信息

Rydz Joanna, Duale Khadar, Musioł Marta, Janeczek Henryk, Hercog Anna, Marcinkowski Andrzej, Molnar Kristof, Michel Frederick C, Klingman Michael, Focarete Maria Letizia, Puskas Judit E, Mielczarek Przemysław, Suder Piotr, El Fray Miroslawa, Walkowiak Konrad, Rokicka Joanna, Niedźwiedź Malwina, Grundmann Alexander, Kaysser Simon T, Detjen Sönke, Johnston Brian, Radecka Iza, Kannappan Vinodh, Kowalczuk Marek

机构信息

Centre of Polymer and Carbon Materials Polish Academy of Sciences, M. Curie-Skłodowskiej 34, Zabrze 41-819, Poland.

SPIN-Lab Centre for Microscopic Research on Matter, University of Silesia in Katowice, 75 Pułku Piechoty 1A, Chorzów 41-500, Poland.

出版信息

ACS Sustain Chem Eng. 2025 Sep 2;13(36):14873-14892. doi: 10.1021/acssuschemeng.5c04602. eCollection 2025 Sep 15.

Abstract

This study explores the integration of triglycine, an oligopeptide, as a green molecular marker in 3D-printed poly-(1,4-butylene adipate--1,4-butylene terephthalate)/polylactide (PBAT/PLA)-based specimens with different printing temperatures to enhance the traceability of (bio)-degradable polymers. This approach supports the advancement of sustainable materials by enabling the identification of the material origin and degradation processes. The research assesses the behavior of the labeled polymer under UV exposure, evaluating the stability of the oligopeptide marker to ensure that the information remains retrievable even after exposure to environmental stressors. In addition, their behavior during aerobic composting, as well as anaerobic digestion, is investigated to promote environmentally friendly practices. This study employed an extraction procedure to isolate and retrieve encoded information, which was then analyzed using a mass spectrometry method, ESI/TIMS-Q-TOF. This makes it possible to determine the sequence of the oligopeptide and compare it with the previously used MALDI-TOF/TOF mass spectrometry procedure. Cytotoxicity studies were also conducted to assess the potential hazards associated with PBAT/PLA-based specimens, considering their potential biomedical applications. The PBAT/PLA-based specimens demonstrated good oligopeptide stability, enabling effective retrieval of recorded information from the green polymer/oligopeptide system even after UV exposure. UV irradiation affected cold crystallization temperature and melting temperature and caused self-chain/cross-linking of the PBAT/PLA-based specimens. In general, the analyses show that specimens printed at a higher temperature (190 °C) have a higher degradation rate than those printed at a lower temperature (155 °C). This phenomenon was attributed to the higher porosity and increased water permeability of the specimens printed at 190 °C, compared to those printed at 155 °C, which is likely due to the greater phase separation and reduced miscibility in the former.

摘要

本研究探索了将一种寡肽——三甘氨酸作为绿色分子标记物整合到具有不同打印温度的3D打印聚(己二酸丁二醇酯-对苯二甲酸丁二醇酯)/聚乳酸(PBAT/PLA)基试样中,以提高(生物)可降解聚合物的可追溯性。这种方法通过能够识别材料来源和降解过程,支持了可持续材料的发展。该研究评估了标记聚合物在紫外线照射下的行为,评估了寡肽标记物的稳定性,以确保即使在暴露于环境应激源后信息仍可检索。此外,还研究了它们在好氧堆肥以及厌氧消化过程中的行为,以促进环境友好型做法。本研究采用了一种提取程序来分离和检索编码信息,然后使用质谱方法ESI/TIMS-Q-TOF进行分析。这使得确定寡肽的序列并将其与先前使用的MALDI-TOF/TOF质谱程序进行比较成为可能。还进行了细胞毒性研究,以评估基于PBAT/PLA的试样的潜在危害,考虑到它们潜在的生物医学应用。基于PBAT/PLA的试样表现出良好的寡肽稳定性,即使在紫外线照射后也能有效地从绿色聚合物/寡肽系统中检索记录的信息。紫外线辐射影响了冷结晶温度和熔点,并导致基于PBAT/PLA的试样发生自链/交联。一般来说,分析表明,在较高温度(190°C)下打印的试样比在较低温度(155°C)下打印的试样具有更高的降解率。这种现象归因于在190°C下打印的试样与在155°C下打印的试样相比具有更高的孔隙率和增加的水渗透性,这可能是由于前者更大的相分离和更低的混溶性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e6a6/12442224/8d93c1b5fa7f/sc5c04602_0020.jpg

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