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A Simple and Cost-Effective FeCl3-Catalyzed Functionalization of Cellulose Nanofibrils: Toward Adhesive Nanocomposite Materials for Medical Implants
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-05-30 , DOI: 10.1021/acsami.4c04351 Evgenii Tikhomirov 1 , Antonio Franconetti 2 , Mathias Johansson 3 , Corine Sandström 3 , Elin Carlsson 4 , Brittmarie Andersson 4 , Nils P Hailer 4 , Natalia Ferraz 1 , Carlos Palo-Nieto 1, 4
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-05-30 , DOI: 10.1021/acsami.4c04351 Evgenii Tikhomirov 1 , Antonio Franconetti 2 , Mathias Johansson 3 , Corine Sandström 3 , Elin Carlsson 4 , Brittmarie Andersson 4 , Nils P Hailer 4 , Natalia Ferraz 1 , Carlos Palo-Nieto 1, 4
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In the present work, we explored Lewis acid catalysis, via FeCl3, for the heterogeneous surface functionalization of cellulose nanofibrils (CNFs). This approach, characterized by its simplicity and efficiency, facilitates the amidation of nonactivated carboxylic acids in carboxymethylated cellulose nanofibrils (c-CNF). Following the optimization of reaction conditions, we successfully introduced amine-containing polymers, such as polyethylenimine and Jeffamine, onto nanofibers. This introduction significantly enhanced the physicochemical properties of the CNF-based materials, resulting in improved characteristics such as adhesiveness and thermal stability. Reaction mechanistic investigations suggested that endocyclic oxygen of cellulose finely stabilizes the transition state required for further functionalization. Notably, a nanocomposite, containing CNF and a branched low molecular weight polyethylenimine (CNF-PEI 800), was synthesized using the catalytic reaction. The composite CNF-PEI 800 was thoroughly characterized having in mind its potential application as coating biomaterial for medical implants. The resulting CNF-PEI 800 hydrogel exhibits adhesive properties, which complement the established antibacterial qualities of polyethylenimine. Furthermore, CNF-PEI 800 demonstrates its ability to support the proliferation and differentiation of primary human osteoblasts over a period of 7 days.
中文翻译：
一种简单且经济有效的 FeCl3 催化的纤维素纳米原纤维功能化：用于医疗植入物的粘合纳米复合材料
在目前的工作中，我们通过 FeCl 3探索了路易斯酸催化，用于纤维素纳米原纤维（CNF）的异质表面功能化。这种方法以其简单和高效为特点，促进了羧甲基化纤维素纳米原纤维（c-CNF）中非活化羧酸的酰胺化。经过优化反应条件，我们成功地将聚乙烯亚胺和Jeffamine等含胺聚合物引入到纳米纤维上。这一引入显着增强了 CNF 基材料的物理化学性质，从而改善了粘合性和热稳定性等特性。反应机理研究表明，纤维素的环内氧可以很好地稳定进一步功能化所需的过渡态。值得注意的是，利用催化反应合成了含有 CNF 和支化低分子量聚乙烯亚胺 (CNF-PEI 800) 的纳米复合材料。考虑到复合材料 CNF-PEI 800 作为医疗植入物涂层生物材料的潜在应用，对其进行了彻底的表征。由此产生的 CNF-PEI 800 水凝胶具有粘合特性，补充了聚乙烯亚胺已确立的抗菌特性。此外，CNF-PEI 800 还展示了其在 7 天内支持原代人成骨细胞增殖和分化的能力。
更新日期：2024-05-30
中文翻译：
一种简单且经济有效的 FeCl3 催化的纤维素纳米原纤维功能化：用于医疗植入物的粘合纳米复合材料
在目前的工作中，我们通过 FeCl 3探索了路易斯酸催化，用于纤维素纳米原纤维（CNF）的异质表面功能化。这种方法以其简单和高效为特点，促进了羧甲基化纤维素纳米原纤维（c-CNF）中非活化羧酸的酰胺化。经过优化反应条件，我们成功地将聚乙烯亚胺和Jeffamine等含胺聚合物引入到纳米纤维上。这一引入显着增强了 CNF 基材料的物理化学性质，从而改善了粘合性和热稳定性等特性。反应机理研究表明，纤维素的环内氧可以很好地稳定进一步功能化所需的过渡态。值得注意的是，利用催化反应合成了含有 CNF 和支化低分子量聚乙烯亚胺 (CNF-PEI 800) 的纳米复合材料。考虑到复合材料 CNF-PEI 800 作为医疗植入物涂层生物材料的潜在应用，对其进行了彻底的表征。由此产生的 CNF-PEI 800 水凝胶具有粘合特性，补充了聚乙烯亚胺已确立的抗菌特性。此外，CNF-PEI 800 还展示了其在 7 天内支持原代人成骨细胞增殖和分化的能力。
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