Elucidating Structural Variations at Heterogeneous Interfaces in Polymer Blends Using Evolved Gas Analysis with Time-of-Flight Mass Spectrometry Under Field Ionization

IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL
Ryota Watanabe*, Taiki Ozawa, Mayumi Kishi and Sayaka Nakamura, 
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Abstract

We present a novel method, viz., evolved gas analysis with time-of-flight mass spectrometry (EGA-TOFMS) using field ionization, for analyzing the molecular-scale structural variations at heterogeneous interfaces in polymer blends. EGA-TOFMS enables the acquisition of temperature-dependent high-resolution mass spectra of the pyrolysis products derived from each component of the blends. However, the inherent complexities of these spectra make their interpretation significantly challenging. To address this issue, we developed a filtered Kendric Mass Defect (filtered KMD) technique that selectively isolates signals corresponding to the pyrolysis products of individual components. Additionally, the elected ion current curve, constructed by summing the ion intensities identified using filtered KMD, was used to analyze the pyrolysis behavior of each component. The utility of these techniques is demonstrated using a ternary polymer blend composed of polypropylene (PP), polyamide 6 (PA6), and a maleic anhydride-grafted styrene–ethylene butylene–styrene triblock copolymer (MASEBS), denoted as PP/PA6/MASEBS. Pyrolysis product analysis revealed that MASEBS chemically interacts with PA6, effectively functioning as a compatibilizer. Incorporating 1 wt % MASEBS enhanced the interfacial compatibility and mechanical properties of PP/PA6/MASEBS, whereas higher loadings resulted in the accumulation of excess unreacted MASEBS, reducing the performance. Our analytical framework offers insights into the structure–property relationships of complex polymer systems.

Abstract Image

利用场电离下的飞行时间质谱分析解析聚合物共混物中非均相界面的结构变化。
我们提出了一种新的方法,即利用场电离的飞行时间质谱(EGA-TOFMS)进行演化气体分析,用于分析聚合物共混物中非均相界面的分子尺度结构变化。EGA-TOFMS能够获得由混合物的每个组分衍生的热解产物的温度依赖的高分辨率质谱。然而,这些光谱的固有复杂性使得它们的解释具有很大的挑战性。为了解决这个问题,我们开发了一种过滤肯德里克质量缺陷(filtered Kendric Mass Defect,过滤KMD)技术,可以选择性地分离出与单个组分热解产物相对应的信号。此外,通过对过滤后的KMD识别的离子强度进行求和,构建了选出的离子流曲线,用于分析各组分的热解行为。用聚丙烯(PP)、聚酰胺6 (PA6)和马来酸酐接枝的苯乙烯-乙烯丁烯-苯乙烯三嵌段共聚物(MASEBS)组成的三元共混聚合物(记为PP/PA6/MASEBS)证明了这些技术的实用性。热解产物分析表明,MASEBS与PA6发生化学反应,有效地发挥增容剂的作用。加入1 wt %的MASEBS可以增强PP/PA6/MASEBS的界面相容性和机械性能,而更高的负载会导致过量未反应MASEBS的积累,从而降低性能。我们的分析框架提供了对复杂聚合物系统的结构-性能关系的见解。
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来源期刊
Analytical Chemistry
Analytical Chemistry 化学-分析化学
CiteScore
12.10
自引率
12.20%
发文量
1949
审稿时长
1.4 months
期刊介绍: Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.
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