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通过电化学氧化制备的高电荷纤维素纳米晶体

Highly Charged Cellulose Nanocrystals via Electrochemical Oxidation.

作者信息

Yousefi Neptun, Hannonen Jenna, Fliri Lukas, Peljo Pekka, Kontturi Eero

机构信息

Department of Bioproducts and Biosystems, Aalto University, P.O. Box 16300, 00076 Aalto, Finland.

Battery Materials and Technologies, Department of Mechanical and Materials Engineering, University of Turku, FI-20014 Turun yliopisto, Finland.

出版信息

Nano Lett. 2024 Nov 20;24(46):14610-14614. doi: 10.1021/acs.nanolett.4c02918. Epub 2024 Nov 6.

DOI:10.1021/acs.nanolett.4c02918
PMID:39505324
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11583315/
Abstract

Due to their exceptional properties, cellulose nanocrystals (CNCs) have been proposed for various applications in sustainable materials science. However, state-of-the-art production methods suffer from low yields and rely on hazardous and environmentally harmful chemicals, representing a bottleneck for more widespread utilization of CNCs. In this study, we present a novel two-step approach that combines previously established HCl gas hydrolysis with electrochemical TEMPO oxidation. This unique method allows the collection of easily dispersible CNCs with high carboxylate contents in excellent overall yields of 71%. The electromediated oxidation was conducted in aqueous conditions without the usually required cocatalysts, simplifying the purification of the materials. Moreover, the proposed process is designed for facile recycling of the used reagents in both steps. To evaluate the sustainability and scalability, the environmental impact factor was calculated, and a cost analysis was conducted.

摘要

由于其优异的性能,纤维素纳米晶体(CNCs)已被提议用于可持续材料科学的各种应用中。然而,目前的生产方法产量低,且依赖于危险和对环境有害的化学品,这是CNCs更广泛应用的一个瓶颈。在本研究中,我们提出了一种新颖的两步法,该方法将先前建立的HCl气体水解与电化学TEMPO氧化相结合。这种独特的方法能够以71%的优异总产率收集具有高羧酸盐含量且易于分散的CNCs。电介导氧化在水性条件下进行,无需通常所需的助催化剂,简化了材料的纯化过程。此外,所提出的工艺设计用于在两个步骤中方便地回收使用过的试剂。为了评估可持续性和可扩展性,计算了环境影响因子并进行了成本分析。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/f4d2f3a1acd9/nl4c02918_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/ab612e3f3cca/nl4c02918_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/d5cfd160650f/nl4c02918_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/7fb33a1a7b2d/nl4c02918_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/a203793a03d3/nl4c02918_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/f4d2f3a1acd9/nl4c02918_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/ab612e3f3cca/nl4c02918_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/d5cfd160650f/nl4c02918_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/7fb33a1a7b2d/nl4c02918_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/a203793a03d3/nl4c02918_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a30c/11583315/f4d2f3a1acd9/nl4c02918_0005.jpg

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本文引用的文献

1
Debugging periodate oxidation of cellulose: Why following the common protocol of quenching excess periodate with glycol is a bad idea.调试过碘酸盐氧化纤维素:为什么按照常规方法用乙二醇淬灭过量的过碘酸盐是不可取的。
Carbohydr Polym. 2023 Jun 15;310:120691. doi: 10.1016/j.carbpol.2023.120691. Epub 2023 Feb 18.
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Efficient Isolation Method for Highly Charged Phosphorylated Cellulose Nanocrystals.高效分离带高电荷的磷酸化纤维素纳米晶的方法。
Biomacromolecules. 2023 Mar 13;24(3):1318-1328. doi: 10.1021/acs.biomac.2c01363. Epub 2023 Feb 7.
3
Integrating direct reuse and extraction recovery of TEMPO for production of cellulose nanofibrils.
整合 TEMPO 的直接再利用和提取回收以生产纤维素纳米纤维。
Carbohydr Polym. 2022 Oct 15;294:119803. doi: 10.1016/j.carbpol.2022.119803. Epub 2022 Jul 1.
4
Cellulose nanocrystals: Fundamentals and biomedical applications.纤维素纳米晶:基础与生物医学应用。
Carbohydr Polym. 2022 Jan 1;275:118668. doi: 10.1016/j.carbpol.2021.118668. Epub 2021 Sep 14.
5
Nanocellulose in biomedical and biosensing applications: A review.纳米纤维素在生物医学和生物传感应用中的研究进展综述
Int J Biol Macromol. 2021 Jan 1;166:587-600. doi: 10.1016/j.ijbiomac.2020.10.217. Epub 2020 Oct 29.
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Recent Developments in Cellulose Nanomaterial Composites.纤维素纳米材料复合材料的最新进展。
Adv Mater. 2021 Jul;33(28):e2000718. doi: 10.1002/adma.202000718. Epub 2020 Jul 21.
7
Native Structure of the Plant Cell Wall Utilized for Top-Down Assembly of Aligned Cellulose Nanocrystals into Micrometer-Sized Nanoporous Particles.用于自上而下组装纤维素纳米晶为微米级纳米多孔颗粒的植物细胞壁的天然结构。
Macromol Rapid Commun. 2020 Aug;41(15):e2000201. doi: 10.1002/marc.202000201. Epub 2020 Jul 1.
8
The Shape of Native Plant Cellulose Microfibrils.天然植物纤维素微纤丝的形态。
Sci Rep. 2018 Sep 18;8(1):13983. doi: 10.1038/s41598-018-32211-w.
9
Cellulose nanocrystals by acid vapour: towards more effortless isolation of cellulose nanocrystals.酸蒸汽法制备纤维素纳米晶体:更轻松地分离纤维素纳米晶体。
Faraday Discuss. 2017 Sep 21;202:315-330. doi: 10.1039/c7fd00053g.
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Degradation and Crystallization of Cellulose in Hydrogen Chloride Vapor for High-Yield Isolation of Cellulose Nanocrystals.在氯化氢蒸汽中降解和结晶纤维素以高产率分离纤维素纳米晶。
Angew Chem Int Ed Engl. 2016 Nov 7;55(46):14455-14458. doi: 10.1002/anie.201606626. Epub 2016 Oct 20.