Polymer Degradation and Stability最新文献_第2页

Disintegration of commercial single-use plastics from synthetic and biobased origins and effects on plant growth 源于合成和生物的一次性商用塑料的分解及其对植物生长的影响

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-11-02 DOI: 10.1016/j.polymdegradstab.2024.111071

Alma Berenice Jasso-Salcedo , Myrna Salinas-Hernández , Abril Fonseca-García , Enrique Javier Jiménez-Regalado , Rocio Yaneli Aguirre-Loredo

Many single–use plastic (SUP) options made of synthetic polymers, bio-based materials, and blends of both are available in the market and used in large quantities. The disintegration of eleven commercial SUP, marketed in Mexico as cups and plates, was investigated in an aerobic home compost environment at a laboratory scale over 180 days. An evaluation of chemical changes, surface morphology, and thermal and mechanical properties was conducted to ascertain the original composition of SUP and the progression of disintegration in samples that are challenging to clean from soil contamination. Furthermore, the impact of residual compost on barley (Hordeum vulgare) plant growth and its correlation with the leaching of heavy metals were explored. The bio-based SUP, but not those made of expanded polystyrene foam, showed a correlation between the disintegration degree (measured by weight loss into particles <2 mm) and a decrease in functional groups (observed by FT-IR), mechanical-thermal stability loss, and surface wear over disintegration time. For instance, the highest disintegration at 180 days was approximately 70 % for wheat bran and palm leaf plates, followed by wheat plates and cellulose-PLA cups (60 %). In addition to the components listed by the manufacturers, the FT-IR and DSC analysis revealed the presence of polyethylene and polypropylene in cellulose cups and sugarcane plates. These components, impede disintegration but contribute to preserving thermal resistance and hydrophobicity during utilization. Compost derived from expanded polystyrene foam SUP, with 90 days of disintegration, was rich in zinc and chromium and significantly decrease in the root length of the barley plant compared to the control. This demonstrates the necessity of considering the impact of the leaching of additives and secondary microplastics into the environment.

市场上有许多由合成聚合物、生物基材料以及两者的混合物制成的一次性塑料（SUP），并被大量使用。在实验室规模的有氧家庭堆肥环境中，对墨西哥市场上销售的 11 种商用杯盘一次性塑料的分解情况进行了 180 天的调查。对化学变化、表面形态以及热和机械性能进行了评估，以确定 SUP 的原始成分以及难以从土壤污染中清除的样品的分解过程。此外，还探讨了残留堆肥对大麦（Hordeum vulgare）植物生长的影响及其与重金属沥滤的相关性。生物基 SUP（而非发泡聚苯乙烯制成的 SUP）的崩解度（以重量损失为 2 毫米的颗粒来衡量）与功能基团的减少（通过傅立叶变换红外光谱观察）、机械热稳定性的降低以及崩解时间的表面磨损之间存在相关性。例如，180 天时，麦麸和棕榈叶板的崩解率最高，约为 70%，其次是小麦板和纤维素-聚乳酸杯（60%）。除了制造商列出的成分外，傅立叶变换红外光谱和 DSC 分析还显示纤维素杯和甘蔗板中含有聚乙烯和聚丙烯。这些成分会阻碍分解，但有助于在使用过程中保持耐热性和疏水性。由发泡聚苯乙烯泡沫 SUP 制成的堆肥在 90 天的分解过程中富含锌和铬，与对照组相比，大麦植株的根长明显减少。这表明有必要考虑添加剂和二次微塑料沥滤对环境的影响。

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引用次数: 0

A flame retardant coating based on amino acid and phytic acid for cotton fabrics 基于氨基酸和植酸的棉织物阻燃涂层

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-11-01 DOI: 10.1016/j.polymdegradstab.2024.111069

Xiao-Hui Shi , Cheng-Yue Jing , Huan Luo , Hong Shi , De-Yi Wang

The effective and eco-friendliness flame retardants for fabrics are increasingly being prioritized. In this study, cotton fabrics were coated with dimethyl phosphite lysine (LP) and phytic acid (PA) to create an eco-friendly and high-efficient fireproof barrier through strong electrostatic attraction and hydrogen bond assembly. The flame-retardant property of the coated cotton fabrics (C/LP10/PA) demonstrated a significant improvement, as evidenced by a limiting oxygen index of 40.2 % and an inherent ability to self-extinguish upon removal of the fire source during vertical burning tests. Furthermore, the synergistic flame-retardant effect of LP and PA resulted in a reduction of 74 % in peak heat release rate and 21 % in total heat release for C/LP10/PA compared to pure cotton. However, the smoke release of C/LP10/PA was increased due to the incomplete combustion. Moreover, the charring process was significantly enhanced in C/LP10/PA with a char residue weight percentage of 26.0 %, from 7.0 % for pure cotton fabric. The analysis of residual char after burning and gaseous products generated during the decomposition process demonstrated that LP/PA coating exhibited flame-retardant properties in both condensed and gas phases. Generally, this work presents a feasible and eco-friendly method for achieving flame retardancy in cotton fabrics.

高效、环保的织物阻燃剂越来越受到重视。本研究在棉织物上涂覆了二甲基亚磷酸酯赖氨酸（LP）和植酸（PA），通过强静电吸引和氢键组装形成了环保高效的防火屏障。在垂直燃烧测试中，涂层棉织物（C/LP10/PA）的阻燃性能得到了显著改善，极限氧指数达到 40.2%，并且在移除火源后具有自熄能力。此外，与纯棉相比，LP 和 PA 的协同阻燃效果使 C/LP10/PA 的峰值热释放率降低了 74%，总热释放率降低了 21%。然而，由于燃烧不完全，C/LP10/PA 的烟雾释放量有所增加。此外，C/LP10/PA 的炭化过程显著增强，残炭重量百分比从纯棉织物的 7.0% 提高到 26.0%。对燃烧后的残炭和分解过程中产生的气态产物的分析表明，LP/PA 涂层在凝结相和气相中都具有阻燃性能。总体而言，这项研究提出了一种实现棉织物阻燃的可行且环保的方法。

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引用次数: 0

Synthesis and properties of poly (alkylene trans-1,4-cyclohexanedicarboxylate)s with different glycolic subunits 具有不同乙醇亚基的聚（反式-1,4-环己烷二甲酸烯丙酯）的合成及其特性

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-31 DOI: 10.1016/j.polymdegradstab.2024.111050

Giulia Guidotti , Clément Fosse , Michelina Soccio , Massimo Gazzano , Valentina Siracusa , Laurent Delbreilh , Antonella Esposito , Nadia Lotti

This work explores one of the numerous playgrounds offered by polyesters. A series of poly (alkylene trans-1,4-cyclohexanedicarboxylate)s were synthesized combining trans-1,4-cyclohexane dicarboxylic acid with four diols containing an increasing number of methylene groups (

n_{{CH}_{2}}

= 3, 4, 5 and 6). The resulting polyesters are fully aliphatic. Their backbones contain cyclic aliphatic moieties and linear aliphatic segments in different relative contents depending on

n_{{CH}_{2}}

. The flexibility of these polyesters can be finely tuned (

T_{g}

decreases proportionally to the increase in

n_{{CH}_{2}}

), however the microstructure dramatically changes depending on whether

n_{{CH}_{2}}

is an odd or an even number (odd-even effect). On one hand, the odd-numbered samples are easier to melt-quench to a fully amorphous glassy state; on the other hand, the even-numbered samples are prone to crystallization and crystallize very fast. The developed microstructure is complex because of the probable coexistence of different crystalline structures, mesophases, and molecular arrangements depending on the cis/trans isomerism of the cyclohexane moiety. Preliminary tests provided mechanical and barrier properties that could make these polyesters suitable for packaging applications. Composting tests showed that increasing

n_{{CH}_{2}}

could eventually improve the biodegradation rate of these polyesters, although crystallinity remains the most influencing parameter.

这项研究探索了聚酯的众多应用领域之一。研究人员将反式-1,4-环己烷二羧酸与四种含有越来越多亚甲基（nCH2 = 3、4、5 和 6）的二元醇结合，合成了一系列聚（反式-1,4-环己烷二羧酸亚烷基酯）。由此产生的聚酯是完全脂肪族的。它们的骨架含有环状脂肪族分子和线性脂肪族段，其相对含量因 nCH2 而异。这些聚酯的柔韧性可以进行微调（Tg 随 nCH2 的增加而成正比地降低），但微观结构会因 nCH2 是奇数还是偶数而发生显著变化（奇偶效应）。一方面，奇数样品更容易熔淬成完全无定形的玻璃态；另一方面，偶数样品容易结晶，而且结晶速度非常快。由于环己烷分子的顺/反异构性不同，可能同时存在不同的结晶结构、介相和分子排列，因此形成的微观结构非常复杂。初步测试表明，这些聚酯具有机械和阻隔性能，可用于包装应用。堆肥试验表明，尽管结晶度仍然是影响最大的参数，但增加 nCH2 最终可提高这些聚酯的生物降解率。

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引用次数: 0

Liquid phosphorus-based bis-imidazole compounds as latent curing agents for enhancing thermal, mechanical, and flame-retardant performances of single-component epoxy resins 液态磷基双咪唑化合物作为潜伏固化剂，用于提高单组分环氧树脂的热性能、机械性能和阻燃性能

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-30 DOI: 10.1016/j.polymdegradstab.2024.111066

Jingsheng Wang , Jun Wang , Fengyi Wang , Shuang Yang , Chaoqun Wu , Xi Chen , Kaiwen Chen , Pingan Song , Hao Wang , Siqi Huo

The escalating need for advanced, fire-resistant, single-component epoxy resin (EP) is fueled by its practicality and economic benefits, highlighting the necessity for the development of multifunctional flame-retardant latent curing agents. Herein, two liquid phosphorus-containing bis-imidazole compounds, PPDM and DPCMI, were synthesized as latent curing agents for EP, demonstrating multiple effects in improving latency, thermal stability, mechanical properties, and fire safety. EP/PPDM and EP/DPCMI showcased superior storage stability and rapid curing at moderate temperatures, with EP/PPDM standing out for its long shelf life of 7 d and being gelled within 18 min at 100 °C. The resulting thermosets presented increased glass transition temperatures (189.5 and 178.9 °C), due to the enhanced crosslinking densities. The presence of bis-imidazole groups in PPDM and DPCMI enabled EPs to form denser crosslinked networks, leading to improved mechanical strength and toughness. The limiting oxygen index (LOI) values of EP/PPDM and EP/DPCMI reached 29.5% and 29.0%, respectively. Compared to the control EP, EP/PPDM and EP/DPCMI showed 23.1% and 18.8% reductions in total heat release and 22.0% and 23.11% decreases in total smoke production. These results confirm the enhanced flame retardancy and smoke suppression of EP/PPDM and EP/DPCMI because of introducing phosphorus-containing groups. Even though the curing time was halved to 2.5 hours, EP/PPDM systems maintained satisfactory overall performances. Therefore, this work offers a scalable strategy for the fabrication of single-component EP systems combining rapid curing, satisfactory flame retardancy, and enhanced thermal stability and mechanical properties, aligning with the needs of industrial applications.

由于单组分环氧树脂（EP）的实用性和经济效益，人们对先进的阻燃单组分环氧树脂（EP）的需求与日俱增，这凸显了开发多功能阻燃潜伏固化剂的必要性。本文合成了两种液态含磷双咪唑化合物 PPDM 和 DPCMI，作为 EP 的潜伏固化剂，在改善潜伏期、热稳定性、机械性能和防火安全方面表现出多重效果。EP/PPDM 和 EP/DPCMI 具有优异的贮存稳定性，并能在中等温度下快速固化，其中 EP/PPDM 尤为突出，它的保质期长达 7 天，并能在 100 °C 下 18 分钟内胶凝。由于交联密度的提高，所产生的热固性材料的玻璃化转变温度也有所提高（分别为 189.5 和 178.9 °C）。PPDM 和 DPCMI 中双咪唑基团的存在使 EPs 能够形成更致密的交联网络，从而提高了机械强度和韧性。EP/PPDM 和 EP/DPCMI 的极限氧指数（LOI）值分别达到 29.5% 和 29.0%。与对照 EP 相比，EP/PPDM 和 EP/DPCMI 的总放热量分别减少了 23.1% 和 18.8%，总产烟量分别减少了 22.0% 和 23.11%。这些结果证实，由于引入了含磷基团，EP/PPDM 和 EP/DPCMI 的阻燃性和抑烟性得到了增强。即使固化时间减半至 2.5 小时，EP/PPDM 系统仍能保持令人满意的总体性能。因此，这项工作为制造单组分 EP 系统提供了一种可扩展的策略，该系统兼具快速固化、令人满意的阻燃性、更高的热稳定性和机械性能，符合工业应用的需求。

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引用次数: 0

Effect of temperature and relative humidity on hydrolytic degradation of additively manufactured PLA: Characterization and artificial neural network modeling 温度和相对湿度对加成制造聚乳酸水解降解的影响：表征和人工神经网络建模

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-28 DOI: 10.1016/j.polymdegradstab.2024.111055

Suha Lee , Jung-Wook Wee

Understanding the long-term durability of 3D-printed polymeric materials under varying temperature and humidity conditions is essential for expanding their industrial applications. Therefore, it is critical to assess the impact of degradation on mechanical properties such as tensile strength. In this study, we manufactured specimens with dual orientations by additive manufacturing-based 3D printing and subjected them to accelerated degradation under various temperature and humidity conditions to evaluate their durability in degradation environments. Mechanical properties significantly decreased under the most severe conditions, with a maximum reduction of 76.7 % observed in molecular weight. The deconvolution of the molecular weight distribution and its correlation with mechanical properties were thoroughly investigated. We derived an equation representing the relationship between the peaks obtained from deconvoluting the molecular weight distribution and the tensile strength. Furthermore, to expedite and simplify tensile strength assessment, we trained an artificial neural network (ANN) model using tensile test results to construct a predictive model. The ANN utilized temperature, humidity, printing angle, and time as input data, with tensile strength as the output. Validation of this model demonstrated the capability to predict tensile strength accurately under different temperature and humidity conditions.

了解三维打印聚合物材料在不同温度和湿度条件下的长期耐久性对于扩大其工业应用至关重要。因此，评估降解对拉伸强度等机械性能的影响至关重要。在本研究中，我们通过基于增材制造的三维打印技术制造了具有双重取向的试样，并将其置于各种温度和湿度条件下进行加速降解，以评估其在降解环境中的耐久性。在最恶劣的条件下，机械性能明显下降，分子量最大下降了 76.7%。我们对分子量分布的解卷积及其与机械性能的相关性进行了深入研究。我们得出了表示分子量分布解卷积得到的峰值与拉伸强度之间关系的方程式。此外，为了加快和简化拉伸强度评估，我们使用拉伸测试结果训练了一个人工神经网络（ANN）模型，以构建一个预测模型。人工神经网络将温度、湿度、印刷角度和时间作为输入数据，将拉伸强度作为输出数据。对该模型的验证表明，它能够准确预测不同温度和湿度条件下的拉伸强度。

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引用次数: 0

Biomimetic synthesis of sea urchin-Like MOFs-LDH and ternary synergistic flame retardants to improve the flame retardancy and UV resistance of Polylactic acid 仿生合成海胆状 MOFs-LDH 和三元协同阻燃剂以提高聚乳酸的阻燃性和抗紫外线性能

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-26 DOI: 10.1016/j.polymdegradstab.2024.111052

Yichen Chen , Xiaodong Jin , Wanfu Wang , Wufei Tang , Chenhao Liu , Shibing Sun

In this work, a novel single molecule flame retardant (DT-S) was synthesized through the self-assembly of diethyltriamine penta-(methylphosphonic) acid and sulfanilamide. Additionally, the three-dimensional sea urchin-like layered double hydroxide hollow dodecahedral structure (MOFs-LDH) was etched from a MOF to increase specific surface area and reaction sites. The chemical structures of DT-S and MOFs-LDH were comprehensively characterized. Subsequently, the obtained flame retardants were molten-compounding into PLA matrix. The fire performance of PLA composites was evaluated by limiting oxygen index (LOI), vertical combustion (UL-94), and cone calorimeter tests. Compared with neat PLA sample, the inclusion of 3 % DT-S and 2 % MOFs-LDH led to an increase in the LOI value from 19.9 to 35.0 %, an upgrade in the UL-94 rating from none to V-0, and a reduction in the peak heat release rate from 524.4 to 401.2 kW m⁻². Analysis of the decomposition products of the PLA composites and the observation of char morphology suggested that DT-S and MOFs-LDH took effects in both condensed phase and gas phase. Furthermore, the evaluation of the UV protection performance using a UV–visible near-infrared spectrophotometer indicated an enhancement in the UV protection performance of PLA, achieving an "excellent" level in evaluating UV protection performance (UPF 50+).

本研究通过二乙基三胺五甲基膦酸和磺胺的自组装合成了一种新型单分子阻燃剂（DT-S）。此外，还从 MOF 中蚀刻出三维海胆状层状双氢氧化物中空十二面体结构（MOFs-LDH），以增加比表面积和反应位点。对 DT-S 和 MOFs-LDH 的化学结构进行了全面表征。随后，将得到的阻燃剂熔融复合到聚乳酸基体中。通过极限氧指数（LOI）、垂直燃烧（UL-94）和锥形量热计测试评估了聚乳酸复合材料的阻燃性能。与纯聚乳酸样品相比，加入 3 % DT-S 和 2 % MOFs-LDH 后，LOI 值从 19.9 % 提高到 35.0 %，UL-94 等级从无提高到 V-0，峰值热释放率从 524.4 kW m-2 降低到 401.2 kW m-2。对聚乳酸复合材料分解产物的分析和对焦炭形态的观察表明，DT-S 和 MOFs-LDH 在凝结相和气相中都发挥了作用。此外，使用紫外可见近红外分光光度计进行的紫外线防护性能评估表明，聚乳酸的紫外线防护性能有所提高，在紫外线防护性能评估中达到了 "优秀 "水平（UPF 50+）。

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引用次数: 0

Efficient flame retardancy of polypropylene by cobalt ions doped phytate melamine synergized with expandable graphite 掺杂钴离子的植酸三聚氰胺与可膨胀石墨协同作用可高效阻燃聚丙烯

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-26 DOI: 10.1016/j.polymdegradstab.2024.111054

Ruilong Li , Yao chen , Honglin Lian , Jianbing Guo , Xiaolang Chen , Junliang Li , Yongzhi Meng , Hong Wu

Maintaining a delicate balance between flame retardancy and amount of expandable graphite (EG) in flame retardant polypropylene (PP) is still a formidable challenge, primarily due to the lower flame-retardant efficiency of EG. In order to address this concern, a novel cobalt-doped nanosheet flame retardant (PAMA-Co) was fabricated by a hydrothermal method utilizing phytic acid (PA) and melamine (MA), exhibiting a promising potential in constructing synergistic EG flame retardant PP. Significantly, the incorporation of only 7 wt% PAMA-Co/23 wt% EG system raises the limiting oxygen index (LOI) of PP to 27.3% and UL-94 V0 level, which indicates the excellent synergistic flame-retardant efficiency of PAMA-Co. Furthermore, both the peak heat release rate (PHRR) and the peak smoke production rate (PSPR) of PP composites with 7 wt% PAMA-Co/23 wt% EG are substantially reduced, exhibiting an 81.6% lower PHRR and 87.8% PSPR compared to pure PP. The excellent flame-retardant efficiency is attributed to the following mechanisms: Gas-phase dilution, catalytic cross-linking charring effect, and the suppression of the EG “popcorn effect” of PAMA-Co. In summary, this work not only advances an understanding of flame-retardant mechanisms but also offers a practical, green strategy for enhancing the safety and utility of PP in various applications.

在阻燃聚丙烯（PP）中保持阻燃性和可膨胀石墨（EG）含量之间的微妙平衡仍然是一项艰巨的挑战，这主要是由于 EG 的阻燃效率较低。为了解决这一问题，研究人员利用植酸（PA）和三聚氰胺（MA），通过水热法制备了一种新型掺钴纳米片状阻燃剂（PAMA-Co），在构建协同 EG 阻燃聚丙烯方面展现出了良好的潜力。值得注意的是，仅添加 7 wt% 的 PAMA-Co/23 wt% 的 EG 体系就能将 PP 的极限氧指数（LOI）提高到 27.3%，达到 UL-94 V0 水平，这表明 PAMA-Co 具有优异的协同阻燃性能。此外，含有 7 wt% PAMA-Co/23 wt% EG 的 PP 复合材料的峰值热释放率（PHRR）和峰值烟雾产生率（PSPR）都大幅降低，与纯 PP 相比，PHRR 降低了 81.6%，PSPR 降低了 87.8%。出色的阻燃效率归功于以下机理：气相稀释、催化交联炭化效应以及抑制 PAMA-Co 的 EG "爆米花效应"。总之，这项工作不仅加深了人们对阻燃机理的理解，还为提高聚丙烯在各种应用中的安全性和实用性提供了一种实用的绿色策略。

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引用次数: 0

Radiolabeling for polymers degradation studies: Opportunities and challenges ahead 用于聚合物降解研究的放射性标记：机遇与挑战并存

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-26 DOI: 10.1016/j.polymdegradstab.2024.111053

Sara Adeleh , Roland Bol , Tabea Becker , Sonja Herres-Pawlis , Harry Vereecken , Thomas Pütz

The production of bio-based polymers as replacements for fossil-based ones is becoming increasingly important to the human society due to the decreasing availability of fossil resources combined with rising fuel prices, and their potential to reduce greenhouse gas emissions that are the main cause of climate change. There is strong societal and regulatory pressure for the development of more sustainable biodegradable bioplastics. Viable recycling options are still lacking for many of these plastics. Due to the novelty of biodegradable bioplastics valuable chains, more research is required to reduce technical and economic uncertainties and demonstrate the feasibility and economic competitiveness of them. Therefore, there is an urgent need for technology development and the design of transition paths towards structural changes in polymers establishing local and regional circular production of bioplastics with potential impact on global economies.

It is essential to understand the factors that control the environmental behavior and fate of such bioplastics as well as their impact on ecosystem functioning. Extensive studies with accurate measurement tools and specialized analytical techniques are needed for this purpose. The radiolabeling technique (¹⁴C) allows the quantification of the degradation process of biopolymers by easily being able to distinguish between CO₂ which is produced during degradation polymers and other carbon sources in natural environment.

This review provides an overview of the application of the ¹⁴C-labeling technique in polymer degradation studies that is compared under various conditions. In following, standard methods for ¹⁴C-labeling, as well as its potentials, obstacles, and deficiencies in usage, are also discussed.

由于化石资源的日益减少和燃料价格的不断上涨，生产生物基聚合物作为化石基聚合物的替代品对人类社会越来越重要，而且生物基聚合物具有减少温室气体排放的潜力，而温室气体排放是气候变化的主要原因。开发更具可持续性的可生物降解生物塑料面临着强大的社会和监管压力。许多此类塑料仍然缺乏可行的回收方案。由于生物可降解塑料价值链的新颖性，需要开展更多研究，以减少技术和经济方面的不确定性，并证明其可行性和经济竞争力。因此，迫切需要进行技术开发和设计过渡途径，以实现聚合物结构的改变，建立对全球经济具有潜在影响的地方和区域生物塑料循环生产。为此，需要利用精确的测量工具和专门的分析技术进行广泛研究。本综述概述了 14C 标记技术在聚合物降解研究中的应用，并在不同条件下进行了比较。随后，还讨论了 14C 标记的标准方法及其应用潜力、障碍和不足。

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引用次数: 0

Failure signal of high orientation Poly(L-lactic acid) monofilament for self-expanding stent during lifetime: Disappeared amorphous connections 用于自膨胀支架的高取向聚（L-乳酸）单丝在使用寿命期间的失效信号：消失的无定形连接

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-24 DOI: 10.1016/j.polymdegradstab.2024.111044

Bin Wang, Jinbo Liu, Xue Hu, Chen Zhang, Qingwei Liu, Zhonghua Ni, Gutian Zhao

The premature failure of bioresorbable self-expanding stents for peripheral arterial disease could lead to form thrombosis and threaten patients′ lives. Predicting the time and cause of mechanical and structural failure is crucial to prevent premature failure of implanted stents. Herein, we report a situ accelerated hydrolysis to investigate the degradation properties of self-expanding stents braided by high-performance Poly(L-lactic acid) (PLLA) monofilaments in an accelerated term over a formal long one. Degradation, microstructure, and mechanical properties were comprehensively evaluated to identify key factors of the failure during lifetime. The results show that the upper temperature limit for accelerated hydrolysis is 50 °C. The mechanical properties undergo multiple stages of functional holding, decreasing, and eventual failure. It is attributed to uneven degradation and distribution of crystalline and amorphous regions. Specifically, the disappearance of amorphous chains between fibrils at 6 months leads to mechanical failure. Further disappearance of amorphous chains within fibrils at 18 months results in structural disintegration. Additionally, the degradation behavior of the stents and potential effects of degradation products on vascular tissues are validated for predictive accuracy. These insights provide valuable experimental references for optimizing design and clinical application of PLLA-based self-expanding stents.

治疗外周动脉疾病的生物可吸收自扩张支架过早失效可能导致血栓形成，威胁患者生命。预测机械和结构失效的时间和原因对于防止植入支架过早失效至关重要。在此，我们报告了一种原位加速水解方法，以研究由高性能聚乳酸（PLLA）单丝编织的自扩张支架在正式长期加速条件下的降解特性。对降解、微观结构和机械性能进行了全面评估，以确定寿命期内失效的关键因素。结果表明，加速水解的温度上限为 50 °C。机械性能经历了功能保持、下降和最终失效等多个阶段。这归因于结晶和非晶区域的不均匀降解和分布。具体来说，纤维之间的无定形链在 6 个月后消失，导致机械性能失效。在 18 个月时，纤维内部的无定形链进一步消失，导致结构解体。此外，还验证了支架的降解行为以及降解产物对血管组织的潜在影响，以确保预测的准确性。这些见解为优化基于聚乳酸的自膨胀支架的设计和临床应用提供了宝贵的实验参考。

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引用次数: 0

Sustainable rubber nanocomposites for hydrogen sealings: Impact of carbon nano-onions and bio-based plasticizer 用于氢密封的可持续橡胶纳米复合材料：纳米碳离子和生物基增塑剂的影响

IF 6.3 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability

Pub Date : 2024-10-22 DOI: 10.1016/j.polymdegradstab.2024.111051

Sohail Yasin , Jianfeng Shi , Sheng Ye , Song Yihu , Aman Ullah , Guangzhong Li , Wenzhu Peng , Chaohua Gu

Additives play a crucial role in modifying and enhancing the properties of rubbers, improving mechanical strength, thermal stability, and chemical resistance to make them more suitable for various applications. The rubber industry faces challenges related to high resource consumption and toxic emissions, which are further impacted by the use of performance-enhancing additives. In hydrogen storage systems, tailored additives are required for rubbers to withstand elevated temperatures and high pressures, preventing hydrogen-induced swelling, a major cause of sealing failure. Herein, a novel form of carbonaceous material, carbon nano-onions (CNOs), and the bio-based plasticizer additive epoxidized soybean oil (ESO) are utilized in conventional silica-filled nitrile butadiene rubber (NBR) nanocomposites to develop low-carbon manufacturing high pressure hydrogen resistant O-rings for sealing applications. The results reveal that the incorporation of CNOs increases the crosslinking density (v_c), assisted by ESO, in silica-filled NBR nanocomposites. While the conventional adipate-based plasticizer and ESO were found to be susceptible to high pressure hydrogen exposures, ESO demonstrated sustained compressive sealing properties with increase in von-Mises stress and in elevated thermo-oxidative conditions over time. The results of the life cycle assessment (LCA) recommend ESO for low-carbon manufacturing in rubber processing over conventional plasticizer.

添加剂在改变和增强橡胶性能、提高机械强度、热稳定性和耐化学性，使其更适用于各种应用方面发挥着至关重要的作用。橡胶行业面临着资源消耗大和有毒排放多的挑战，而性能增强添加剂的使用又进一步影响了这些挑战。在储氢系统中，橡胶必须使用定制添加剂才能承受高温高压，防止氢引起的膨胀，这是密封失效的主要原因。在本文中，一种新型碳质材料--碳纳米离子（CNOs）和生物基增塑剂添加剂环氧化大豆油（ESO）被用于传统的二氧化硅填充丁腈橡胶（NBR）纳米复合材料中，从而开发出用于密封应用的低碳、耐高压氢气的 O 型圈。研究结果表明，在二氧化硅填充丁腈橡胶纳米复合材料中，CNO 的加入可在 ESO 的辅助下提高交联密度 (vc)。研究发现，传统的己二酸酯类增塑剂和 ESO 容易受到高压氢气暴露的影响，而 ESO 则能随着 von-Mises 应力的增加和热氧化条件的升高，长期保持压缩密封性能。生命周期评估（LCA）结果表明，ESO 比传统增塑剂更适用于橡胶加工中的低碳制造。

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