高分辨率MALDI-TOF质谱法分析聚(3-羟基丁酸酯-co-3-羟基己酸酯)的单体分布。

IF 2.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL
Naoki Kanayama, Sayaka Nakamura, Shin Sano, Mami Tanaka, Noriko Takahara, Hiroaki Sato and Hideaki Hagihara
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引用次数: 0

摘要

在聚(3-羟基丁酸酯)(PHB)共聚酯的实际应用中,共聚单体单元在聚合物链内的分布(即共聚单体分布)与共聚单体的结构和含量一样,是影响材料各种性能的重要因素。然而,PHB共聚聚酯中共聚单体分布的表征和表征的分析方法仍然有限。在本研究中,我们使用基质辅助激光解吸/电离螺旋飞行时间质谱(maldi -螺旋- tof - ms)检测了聚(3-羟基丁酸-co-3-羟基己酸酯)(PHBH)中的共聚单体分布。高分子量PHBH样品被部分甲醇化,随后通过尺寸排除色谱分离得到合适分子大小的低聚物进行分析。maldi -螺旋- tof - ms的高分辨率能够分离PHBH低聚物中具有相似m/z值的离子峰,并确定其准确的质量。得到的质谱数据随后进行Kendrick质量缺陷(KMD)分析,根据离子峰的端基结构对其进行分类,从而便于识别不同的分子种类。精确的质量测量可以明确地确定PHBH低聚物的相应分子式、端基和单体组成。通过组织特定长度的PHBH链(例如21-mer)对应的离子峰数据,3-羟基己酸酯(3HH)单元在分子链内的分布被表示为该链长度的数字分布图。该分析方法也成功地应用于海水中生物降解的PHBH膜残留物。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Comonomer distribution analysis of poly(3-hydroxybutyrate-co-3-hydroxyhexanoate)s using high-resolution MALDI-TOF mass spectrometry†

Comonomer distribution analysis of poly(3-hydroxybutyrate-co-3-hydroxyhexanoate)s using high-resolution MALDI-TOF mass spectrometry†

In practical applications of poly(3-hydroxybutyrate) (PHB) copolyesters, the distribution of comonomer units within the polymer chains (i.e., comonomer distribution) is an important factor influencing various material properties, alongside the comonomer structure and content. However, analytical methodologies for the characterisation and representation of comonomer distribution in PHB copolyesters remain limited. In the present study, we examined the comonomer distribution in poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBH) using matrix-assisted laser desorption/ionisation spiral time-of-flight mass spectrometry (MALDI-spiral-TOF-MS). High-molecular-weight PHBH samples were partially methanolysed and subsequently fractionated by size-exclusion chromatography to yield oligomers of suitable molecular sizes for analysis. The high-resolution capabilities of MALDI-spiral-TOF-MS enabled the separation of ion peaks with similar m/z values in the PHBH oligomers and the determination of their accurate masses. The resulting mass spectral data were subsequently subjected to Kendrick mass defect (KMD) analysis to classify ion peaks according to their end-group structures, thereby facilitating the identification of distinct molecular species. Accurate mass measurements enabled the unambiguous determination of the corresponding molecular formulae, end groups, and monomer compositions of the PHBH oligomers. By organising the ion peak data corresponding to PHBH chains of a specific length (e.g., 21-mer), the distribution of 3-hydroxyhexanoate (3HH) units within the molecular chain was represented as a number distribution plot for that chain length. This analytical approach was also succesfully applied to PHBH film residues subjected to biodegradation in seawater.

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来源期刊
Analytical Methods
Analytical Methods CHEMISTRY, ANALYTICAL-FOOD SCIENCE & TECHNOLOGY
CiteScore
5.10
自引率
3.20%
发文量
569
审稿时长
1.8 months
期刊介绍: Early applied demonstrations of new analytical methods with clear societal impact
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