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“三维环保型”氨基酸功能化壳聚糖:铀吸附性能及机理研究

"Three-dimensional environment-friendly" amino acid functionalized chitosan: Uranium adsorption performance and mechanism research.

作者信息

Zhu Ruiqi, Zhang Chunhong, Zhu Lien, Liu Lijia, Huo Feng, Wang Yudan, Bai Jianwei, Ma Fuqiu, Dong Hongxing

机构信息

Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, PR China.

Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, PR China; Yantai Research Institute of Harbin Engineering University, Yantai 264006, PR China.

出版信息

Carbohydr Polym. 2024 Nov 1;343:122464. doi: 10.1016/j.carbpol.2024.122464. Epub 2024 Jul 6.

Abstract

To achieve the goals of "carbon peak and carbon neutrality" and sustainable development, we propose "Three-Dimensional Environment-Friendly" materials to balance the urgent need for the development of clean energy and the reduction of secondary environmental pollution during adsorbent preparation. In this study, three novel chitosan adsorbents (CMNSC-Leu, CMNSC-Pro, CMNSC-Phe) for uranium adsorption were designed on the basis of molecular level and successfully synthesized with three different amino acids (leucine, proline, phenylalanine) through amidation reaction in an aqueous environment using a sustainable green chitosan material. The uranium adsorption capacity of the three adsorbents was evaluated by batch adsorption, selectivity and recyclability studies. The adsorption reaction conformed to the pseudo-second-order model and was a spontaneous endothermic reaction. In particular, the maximum adsorption capacity of CMNSC-Pro for uranium was 462.7 mg·g at C = 100 ppm. In addition, CMNSC-Pro showed better selectivity and good reusability. DFT calculation and IRI diagram were applied in this work to analyze the unique structure and adsorption process of CMNSC-Pro from the perspective of structure. Uranium was adsorbed by CMNSC-Pro via coordination, electrostatic interaction, and intraparticle diffusion. This work provided a new idea for the structural design and construction of new high-efficiency biomass adsorbents.

摘要

为实现“碳达峰、碳中和”目标以及可持续发展,我们提出“三维环保”材料,以平衡清洁能源发展的迫切需求与吸附剂制备过程中二次环境污染减少的需求。在本研究中,基于分子水平设计了三种用于铀吸附的新型壳聚糖吸附剂(CMNSC - 亮氨酸、CMNSC - 脯氨酸、CMNSC - 苯丙氨酸),并使用可持续绿色壳聚糖材料在水环境中通过酰胺化反应成功地与三种不同氨基酸(亮氨酸、脯氨酸、苯丙氨酸)合成。通过批量吸附、选择性和可回收性研究评估了这三种吸附剂对铀的吸附能力。吸附反应符合准二级模型,是一个自发吸热反应。特别地,在C = 100 ppm时,CMNSC - 脯氨酸对铀的最大吸附容量为462.7 mg·g 。此外,CMNSC - 脯氨酸表现出更好的选择性和良好的可重复使用性。本工作应用密度泛函理论(DFT)计算和红外光谱(IRI)图从结构角度分析CMNSC - 脯氨酸的独特结构和吸附过程。铀通过配位、静电相互作用和颗粒内扩散被CMNSC - 脯氨酸吸附。这项工作为新型高效生物质吸附剂的结构设计和构建提供了新思路。

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