CAREER: Hierarchical Structures and Tunable Mechanics of Polyelectrolyte Complex-Interpenetrating Network (PEC-IPN) Hydrogels

职业：聚电解质复合互穿网络（PEC-IPN）水凝胶的层次结构和可调力学

• 批准号: 2048285
• 负责人: Samanvaya Srivastava
• 金额: $ 60.65万
• 依托单位: University of California-Los Angeles
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-03-01 至 2026-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2048285&HistoricalAwards=false
• 关键词: CAREER; Hierarchical; Structures; Tunable; Mechanics

NON-TECHNICAL SUMMARY:Hydrogels are water-laden polymer networks with applications in diverse areas including drug delivery, cell and tissue engineering, bioadhesives and tissue sealants and biosensing. This project will create novel types of self-assembled hydrogels composed of two interweaving polymeric networks, with one containing permanent linkages and the other comprising reversible linkages held together by attractive electrostatic interactions among oppositely charged polymers. These new materials will feature complex, hierarchical nanoscale structures and unique elastic, flow and adhesive properties, with relevance in development of the next generation of wet adhesives and tissue sealants. Furthermore, the planned experiments will advance our fundamental understanding of the assembly of charge-containing polymers and the mechanisms through which reversibly-linked networks support the slow, in-situ growth of permanently linked networks. In the broader context, this project will further the understanding and appreciation of polymeric and adhesive materials, polymer physics and chemistry, and advanced material characterization techniques to high school, undergraduate and graduate students through hands-on experiments and demonstrations, new courses and course modules, and regional research symposia, thus motivating the next generation of polymer scientists. In parallel, development of tutorials and interactive software data analysis tools for soft material characterization techniques will contribute to educate and expand the user base of these techniques and serve the broader scientific community.TECHNICAL SUMMARY:Creating hydrogels with controlled cohesive and adhesive properties, during and after curing, remains a challenge. This project will institute design paradigms for creating polyelectrolyte complex-interpenetrating network (PEC-IPN) hydrogels featuring orthogonally tunable bulk and interfacial strengths and toughness. Fundamental studies of self-assembly of oppositely charged block polyelectrolytes into polyelectrolyte complex (PEC) networks will elucidate their hierarchical structure, chain dynamics and mechanical properties, and the evolution of these physical attributes upon inclusion of small molecule or polymeric additives in PEC hydrogels. Crosslinking of diverse chemically crosslinkable monomeric and polymeric precursors, incorporated in PEC hydrogels, will be demonstrated as routes to create PEC-IPN materials with controlled network microstructures. Furthermore, the proposed studies will reveal the enhancements in bulk elasticity and toughness of PEC-IPN hydrogels that emerge from stress dissipation in the self-assembled PEC domains constituting the PEC network. Consequently, PEC-IPN hydrogel adhesives with tuned bulk and interfacial mechanical properties will be developed, targeting potential applications as robust underwater adhesives and tissue sealants. Concurrently, this work will contribute towards establishing a knowledge base for PEC self-assemblies, analogous to the existing base for traditional amphiphilic block polymer assemblies. The proposed research will thus develop a family of versatile self-assembled PEC-based materials that rival yet are distinct from amphiphilic block polymer assemblies and expand the realm of their applications such as micellar drug and gene delivery vehicles..This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

非技术综述：水凝胶是一种含水的聚合物网络，在药物输送、细胞和组织工程、生物粘合剂和组织密封剂以及生物传感等不同领域中都有应用。该项目将创造新型的自组装水凝胶，由两个交织的聚合物网络组成，一个包含永久连接，另一个包含通过相反电荷聚合物之间吸引的静电相互作用而结合在一起的可逆连接。这些新材料将具有复杂的、分级的纳米结构以及独特的弹性、流动和粘合性能，与下一代湿式粘合剂和组织密封剂的开发相关。此外，计划中的实验将促进我们对含电荷聚合物的组装以及可逆连接网络支持永久连接网络的缓慢原位增长的机制的基本理解。在更广泛的背景下，该项目将通过动手实验和演示、新课程和课程模块以及区域研究座谈会，加深高中、本科生和研究生对聚合物和粘性材料、聚合物物理和化学以及先进材料表征技术的理解和欣赏，从而激励下一代聚合物科学家。同时，开发软材料表征技术的教程和交互式软件数据分析工具将有助于教育和扩大这些技术的用户基础，并为更广泛的科学界服务。技术概述：在固化过程中和固化后创造具有受控粘结和粘合性能的水凝胶仍然是一个挑战。该项目将建立创建聚电解质复合互穿网络(PEC-IPN)水凝胶的设计范例，该水凝胶具有正交可调的体积和界面强度和韧性。相反电荷嵌段聚电解质自组装成聚电解质络合物(PEC)网络的基础研究将阐明其层次结构、链动力学和力学性能，以及在PEC水凝胶中加入小分子或聚合物添加剂后这些物理属性的演变。在PEC水凝胶中加入不同的化学可交联性单体和聚合物前驱体的交联性将被证明是创建具有受控网络结构的PEC-IPN材料的途径。此外，拟议的研究将揭示PEC-IPN水凝胶的整体弹性和韧性的增强，这些水凝胶是在构成PEC网络的自组装PEC结构域内的应力消散而产生的。因此，具有可调体积和界面机械性能的PEC-IPN水凝胶粘合剂将被开发出来，目标是作为坚固的水下粘合剂和组织密封剂的潜在应用。同时，这项工作将有助于建立PEC自组装的知识库，类似于传统的两亲性嵌段聚合物组装的现有基础。因此，拟议的研究将开发一系列多功能的自组装PEC基材料，这些材料与两亲性嵌段聚合物组件竞争但又不同，并扩大其应用领域，如胶束药物和基因输送载体。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Polyelectrolyte complex scaffoldings for photocrosslinked hydrogels

用于光交联水凝胶的聚电解质复合支架

• DOI: 10.1039/d2me00171c
• 发表时间: 2023
• 期刊: Molecular Systems Design & Engineering
• 影响因子: 3.6
• 作者: Li, Defu;Ghovvati, Mahsa;Annabi, Nasim;Srivastava, Samanvaya
• 通讯作者: Srivastava, Samanvaya

A user-friendly graphical user interface for dynamic light scattering data analysis

用于动态光散射数据分析的用户友好的图形用户界面

• DOI: 10.1039/d3sm00469d
• 发表时间: 2023
• 期刊: Soft Matter
• 影响因子: 3.4
• 作者: Salazar, Matthew;Srivastav, Harsh;Srivastava, Abhishek;Srivastava, Samanvaya
• 通讯作者: Srivastava, Samanvaya

Comb Polyelectrolytes Stabilize Complex Coacervate Microdroplet Dispersions

• DOI: 10.1021/acsmacrolett.2c00327
• 发表时间: 2022-07-05
• 期刊: ACS MACRO LETTERS
• 影响因子: 7.015
• 作者: Gao, Shang;Srivastava, Samanvaya
• 通讯作者: Srivastava, Samanvaya

Polyelectrolyte Complex-Covalent Interpenetrating Polymer Network Hydrogels

• DOI: 10.1021/acs.macromol.2c00590
• 发表时间: 2022-06-14
• 期刊: MACROMOLECULES
• 影响因子: 5.5
• 作者: Li, Defu;Goeckler, Tobias;Srivastava, Samanvaya
• 通讯作者: Srivastava, Samanvaya