Reducing Hydrophilicity of Cellulose Nanofibrils Through Lipase-Catalyzed Surface Engineering with Renewable Grafting Agents

IF 4.7 3区 工程技术 Q2 ENGINEERING, ENVIRONMENTAL
Guilherme Rezende Costa, Marcus Vinícius Nascimento, Braz de Souza Marotti, Valdeir Arantes
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Abstract

Cellulose nanofibrils are distinguished bionanomaterials known for their unique morphology, thermal stability, and ability to form networks, yet they encounter challenges in compatibility with hydrophobic matrices, limiting their application in various applications. This study introduces an innovative surface modification method to address the high hydrophilicity of CNFs. The novelty lies in the use of lipase as a biocatalyst in combination with renewable grafting agents, specifically butanoic and oleic acids. The lipase successfully esterified both acids onto the CNFs, with butanoic acid exhibiting a higher surface concentration, resulting in a more substantial reduction in hydrophilicity. Contact angle measurements demonstrated a notable shift, from 10.84° for untreated CNF to 68.4° and 55.1° for CNFs grafted with butanoic and oleic acid residues, respectively. While there were only slight alterations in crystallinity, thermal stability, and brittleness, lipase proved to be an effective catalyst for modifying the CNF surface with fatty acids. This approach offers a method to mitigate the high hydrophilicity of CNFs without compromising their key properties. Furthermore, it can be proposed as a means to tailor CNF for water-resistant applications in fields such as electronics, packaging, and Pickering emulsions.

Graphical Abstract

The structure of the lipase protein was sourced from the Protein Data Bank (PDB), first referenced by Xie et al. [38]

Abstract Image

利用可再生接枝剂通过脂肪酶催化表面工程降低纤维素纳米纤维的亲水性
纤维素纳米纤丝是一种杰出的仿生材料,以其独特的形态、热稳定性和形成网络的能力而闻名,但它们在与疏水性基质的兼容性方面遇到了挑战,限制了它们在各种应用中的应用。本研究介绍了一种创新的表面改性方法来解决 CNFs 的高亲水性问题。其新颖之处在于将脂肪酶作为生物催化剂与可再生接枝剂(特别是丁酸和油酸)结合使用。脂肪酶成功地将这两种酸酯化到了 CNF 上,其中丁酸的表面浓度更高,导致亲水性大幅降低。接触角测量结果表明,未处理的 CNF 接触角为 10.84°,而接枝了丁酸和油酸残基的 CNF 接触角分别为 68.4°和 55.1°。虽然结晶度、热稳定性和脆性只有轻微变化,但脂肪酶被证明是用脂肪酸改性 CNF 表面的有效催化剂。这种方法提供了一种在不影响 CNF 关键特性的前提下减轻其高亲水性的方法。此外,它还可作为一种手段,为电子、包装和皮克林乳液等领域的防水应用定制 CNF。图解摘要脂肪酶蛋白质的结构来源于蛋白质数据库(PDB),最早由 Xie 等人引用[38]。
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来源期刊
Journal of Polymers and the Environment
Journal of Polymers and the Environment 工程技术-高分子科学
CiteScore
9.50
自引率
7.50%
发文量
297
审稿时长
9 months
期刊介绍: The Journal of Polymers and the Environment fills the need for an international forum in this diverse and rapidly expanding field. The journal serves a crucial role for the publication of information from a wide range of disciplines and is a central outlet for the publication of high-quality peer-reviewed original papers, review articles and short communications. The journal is intentionally interdisciplinary in regard to contributions and covers the following subjects - polymers, environmentally degradable polymers, and degradation pathways: biological, photochemical, oxidative and hydrolytic; new environmental materials: derived by chemical and biosynthetic routes; environmental blends and composites; developments in processing and reactive processing of environmental polymers; characterization of environmental materials: mechanical, physical, thermal, rheological, morphological, and others; recyclable polymers and plastics recycling environmental testing: in-laboratory simulations, outdoor exposures, and standardization of methodologies; environmental fate: end products and intermediates of biodegradation; microbiology and enzymology of polymer biodegradation; solid-waste management and public legislation specific to environmental polymers; and other related topics.
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