金属复合物光催化剂的配体解离,在动态共价水凝胶中实现 pH 值光电操纵,打印可再加工和可回收设备

IF 5.1 Q1 POLYMER SCIENCE ACS Macro Letters Pub Date : 2024-05-16 DOI:10.1021/acsmacrolett.4c00233
Qian Wang, Zhenhao Zhu, Jupen Liu, Zhe Lu, Yanxia Zhao and You Yu*, 
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引用次数: 0

摘要

动态共价水凝胶因其令人印象深刻的机械性能、仿生结构和动态行为,在智能材料、软设备、电子学等领域的应用潜力正日益受到关注。然而,如何设计精确高效的动态光化学方法来制备动态水凝胶,从而实现复杂的结构和对动态过程的控制,是一项重大挑战。在此,我们提出了一种通用而直接的正交动态共价光化学策略,用于制备高性能可印刷动态共价水凝胶,从而拓宽其先进的应用领域。这种光化学策略使用双功能光催化剂启动自由基聚合,并通过光介导的快速解离机制释放配体。这一过程可在 100 秒内使系统 pH 值从弱酸性受控地升至碱性,进而引发对 pH 值敏感的硼酸/二元醇络合和克努瓦纳格尔缩合模型反应。正交光化学作用可形成相互渗透和连接的网络,显著提高水凝胶的机械性能。在此过程中形成的可逆键,即硼酸酯键和不饱和酮键,可通过光化学 pH 值变化赋予水凝胶优异的自愈合、可再加工和可回收特性。此外,这种快速、可控的制造工艺和动态行为与打印技术高度兼容,从而能够设计出具有不同结构的自适应和可回收传感器。这些进步为各种材料科学、医学和工程应用带来了希望。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Ligand Dissociation of Metal-Complex Photocatalysts toward pH-Photomanipulation in Dynamic Covalent Hydrogels for Printing Reprocessable and Recyclable Devices

Dynamic covalent hydrogels are gaining attention for their potential in smart materials, soft devices, electronics, and more thanks to their impressive mechanical properties, biomimetic structures, and dynamic behavior. However, a significant challenge lies in designing precise and efficient dynamic photochemistry for their preparation, allowing for complex structures and control over the dynamic process. Herein, we propose a general and straightforward orthogonal dynamic covalent photochemistry strategy for preparing high-performance printable dynamic covalent hydrogels, thereby broadening their advanced applications. This photochemical strategy uses a bifunctional photocatalyst to initiate radical polymerization and release ligands through a rapid light-mediated dissociation mechanism. This process leads to a controlled increase in system pH from mildly acidic to alkaline conditions within one hundred seconds, which in turn triggers the pH-sensitive model reactions of boronic acid/diol complexation and Knoevenagel condensation. The orthogonal photochemistry enables the formation of interpenetrated and conjoined networks, significantly enhancing the mechanical properties of the hydrogels. The reversible bonds formed during the process, i.e., boronic ester and unsaturated ketone bonds, confer excellent self-healing, reprocessable, and recyclable properties on the hydrogels through photochemical pH variations. Furthermore, this rapid, controlled fabrication process and dynamic behavior are highly compatible with printing techniques, enabling the design of adaptive and recyclable sensors with different structures. These advancements are promising for various material science, medicine, and engineering applications.

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来源期刊
CiteScore
10.40
自引率
3.40%
发文量
209
审稿时长
1 months
期刊介绍: ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.
期刊最新文献
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