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Crystalline Nanoflowers Derived from the Intramolecular Cyclization-Induced Self-Assembly of an Amorphous Poly(amic acid) at High Solid Content
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-08-15 , DOI: 10.1021/acsmacrolett.4c00472 Jiamei Liu 1 , Tao Wang 1 , Hui Sun 1
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-08-15 , DOI: 10.1021/acsmacrolett.4c00472 Jiamei Liu 1 , Tao Wang 1 , Hui Sun 1
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The investigation of the amorphous to crystalline transformation and the corresponding influence on the self-assembly behavior of amphiphilic polymers are of significant interest in this field. Herein, we propose the concept of intramolecular cyclization-induced self-assembly (ICISA) to prepare crystalline nanoflowers at a high solid content of 15% on the basis of the amorphous to crystalline transformation of poly(amic acid) (PAA). Taking advantage of the reactive property of the PAA, rigid and crystalline polyimide (PI) segments are introduced to the backbone of the PAA to give P(AA-stat-I) induced by the intramolecular cyclization reaction upon thermal treatment, leading to the in situ formation of crystalline nanoflowers. Revealing the formation mechanism of the nanoflowers, we found that the nanosheets are formed at the early stage and then stacked to form the nanoflowers at high concentrations. The relationship between the degree of imidization and incubation temperature is quantitatively analyzed, and the effects of temperature on the morphology, degree of imidization, and crystallinity of the assemblies are also investigated. Furthermore, computer simulations demonstrate the optimized temperature of ICISA of 160 °C, which ensures the match between the intramolecular cyclization reaction rate, the self-assembly process, and the lowest energy state of the self-assembly system, resulting in the formation of nanoflowers with high crystallinity. Overall, a facile one-step strategy is proposed to prepare crystalline nanoflowers based on the in situ thermally triggered intramolecular cyclization reaction of a PAA, which may bring fresh insights into the dynamic amorphous to the crystalline transformation of polymers.
中文翻译：
高固含量非晶态聚酰胺酸分子内环化诱导自组装产生的结晶纳米花
无定形到结晶转变的研究以及对两亲聚合物自组装行为的相应影响是该领域的重要研究内容。在此，我们提出了分子内环化诱导自组装（ICISA）的概念，在聚酰胺酸（PAA）非晶态到晶态转变的基础上制备了15％高固含量的结晶纳米花。利用PAA的反应特性，将刚性的结晶聚酰亚胺（PI）链段引入到PAA的主链中，通过热处理时的分子内环化反应诱导产生P（AA- stat -I），从而产生晶体纳米花的原位形成。揭示纳米花的形成机制，我们发现纳米片在早期形成，然后堆叠形成高浓度的纳米花。定量分析了亚胺化程度与孵育温度之间的关系，并研究了温度对组装体的形貌、亚胺化程度和结晶度的影响。此外，计算机模拟显示ICISA的最佳温度为160℃，保证了分子内环化反应速率、自组装过程和自组装系统最低能态之间的匹配，从而形成纳米花具有高结晶度。总体而言，提出了一种基于PAA原位热触发分子内环化反应制备结晶纳米花的简便一步策略，这可能为聚合物的动态无定形到结晶转变带来新的见解。
更新日期：2024-08-15
中文翻译：
高固含量非晶态聚酰胺酸分子内环化诱导自组装产生的结晶纳米花
无定形到结晶转变的研究以及对两亲聚合物自组装行为的相应影响是该领域的重要研究内容。在此，我们提出了分子内环化诱导自组装（ICISA）的概念，在聚酰胺酸（PAA）非晶态到晶态转变的基础上制备了15％高固含量的结晶纳米花。利用PAA的反应特性，将刚性的结晶聚酰亚胺（PI）链段引入到PAA的主链中，通过热处理时的分子内环化反应诱导产生P（AA- stat -I），从而产生晶体纳米花的原位形成。揭示纳米花的形成机制，我们发现纳米片在早期形成，然后堆叠形成高浓度的纳米花。定量分析了亚胺化程度与孵育温度之间的关系，并研究了温度对组装体的形貌、亚胺化程度和结晶度的影响。此外，计算机模拟显示ICISA的最佳温度为160℃，保证了分子内环化反应速率、自组装过程和自组装系统最低能态之间的匹配，从而形成纳米花具有高结晶度。总体而言，提出了一种基于PAA原位热触发分子内环化反应制备结晶纳米花的简便一步策略，这可能为聚合物的动态无定形到结晶转变带来新的见解。
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