纤维素纳米晶体的羧化通过双交联网络增强和增韧橡胶,ACS Applied Polymer Materials

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纤维素纳米晶体的羧化通过双交联网络增强和增韧橡胶
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2021-11-09 , DOI: 10.1021/acsapm.1c00975
Jie Hu ₁ , Zhengqing Kong ₁ , Ke Liu ₁ , Jinli Qin ₁ , Yuhong Tao ₁ , Lijuan Zhou ₁ , Yuan Yuan ₁ , Min Jiang ₁ , Yongxin Duan ₁ , Jianming Zhang ₁

Affiliation

纤维素纳米晶体 (CNCs) 的表面功能化以及 CNCs 与橡胶基体之间强界面粘附的构建是实现高性能橡胶/CNCs 纳米复合材料的有效途径。在此，磺酸型 CNCs (CNC-OSO ₃ H) 的羧化反应是在水性介质中使用柠檬酸 (CA) 作为改性剂进行的。CNC-OSO ₃ H表面成功接枝了大量羧基，大部分磺酸基被去除，使CNC-OSO ₃羧基化H（缩写为 CNC-CA）具有更高的化学反应性和热稳定性。随后，以聚乙二醇二缩水甘油醚（PEGDE）为交联剂，CNC-CA为增强填料，制备了具有双交联网络的羧化丁苯橡胶（XSBR）/CNC-CA纳米复合材料。傅里叶变换红外光谱研究发现，在所得纳米复合材料中，CNC-CA和XSBR上的羧基相互形成氢键（物理交联），同时羧基与PEGDE上的环氧基形成共价键。物理和化学交联的共存提高了CNC-CA与XSBR基体的界面相容性，加速了CNC-CA的均匀分散，实现了基体本身的交联。正如预期的那样，具有双交联网络的 XSBR/CNC-CA 纳米复合材料在拉伸强度（高达 500%）、模量（高达 151%）和断裂功（高达 348%）方面表现出显着增强。这项工作为获得羧化 CNCs 提供了一种简便、绿色的方法，也为制备具有双交联网络的高性能橡胶纳米复合材料提供了一种方便的方法。

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Carboxylation of Cellulose Nanocrystals for Reinforcing and Toughing Rubber Through Dual Cross-linking Networks

The surface functionalization of cellulose nanocrystals (CNCs) and the construction of strong interfacial adhesion between CNCs and the rubber matrix are effective ways to achieve high-performance rubber/CNCs nanocomposites. Herein, carboxylation of sulfonic CNCs (CNC–OSO₃H) was conducted in an aqueous medium by using citric acid (CA) as the modifier. A large number of carboxyl groups were successfully grafted on the surface of CNC–OSO₃H, and most of the sulfonic groups were removed, which endows the carboxylated CNC–OSO₃H (abbreviated as CNC–CA) with higher chemical reactivity and thermal stability. Subsequently, carboxylated styrene-butadiene rubber (XSBR)/CNC–CA nanocomposites with a dual cross-linking network were prepared by using polyethylene glycol diglycidyl ether (PEGDE) as the cross-linking agent and CNC–CA as reinforcing fillers. Fourier transform infrared spectroscopic investigation found that in the obtained nanocomposites, the carboxyl groups on CNC–CA and XSBR formed hydrogen bonds (physical cross-linking) with each other, and the carboxyl groups formed covalent bonds with the epoxy group on PEGDE simultaneously. The coexistence of physical and chemical cross-linking improved the interface compatibility between CNC–CA and the XSBR matrix, accelerated the homogeneous dispersion of CNC–CA, and realized the cross-linking of the matrix itself. As expected, XSBR/CNC–CA nanocomposites with a dual cross-linking network showed a remarkable enhancement in tensile strength (up to 500%), modulus (up to 151%), and work of fracture (up to 348%). This work provides both a facile and green approach to obtain carboxylated CNCs and a convenient method for the preparation of high-performance rubber nanocomposites with dual cross-linking networks.

更新日期：2021-12-10

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