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用于溶液中高效碘消除的铜功能化、ZIF-8衍生的氮掺杂碳复合材料

Cu-Functionalized, ZIF-8-Derived, Nitrogen-Doped Carbon Composites for Efficient Iodine Elimination in Solution.

作者信息

Chen Jiuyu, Gao Chensheng, Chen Jingwen, Liu Fei, Liu Zhiwen

机构信息

School of Petroleum and Natural Gas Engineering, Changzhou University, Changzhou 213164, China.

Key Laboratory for Protected Agricultural Engineering in the Middle and Lower Reaches of Yangtze River, Institute of Agricultural Facilities and Equipment, Jiangsu Academy of Agricultural Sciences, Ministry of Agriculture and Rural Affairs, Nanjing 210014, China.

出版信息

Nanomaterials (Basel). 2025 Jan 12;15(2):105. doi: 10.3390/nano15020105.

Abstract

The development of copper-based materials with a high efficiency and low cost is desirable for use in iodine (I) remediation. Herein, Cu-nanoparticles-functionalized, ZIF-8 (Zeolite Imidazole Framework-8)-derived, nitrogen-doped carbon composites (Cu@Zn-NC) were synthesized by ball milling and pyrolysis processes. The as-prepared composites were characterized using SEM, BET, XRD, XPS, and FT-IR analyses. The results showed that the morphology of ZIF-8 changed from a leaf-like structure into an irregular structure after the introduction of a copper salt and carbonization. The copper in the pyrolysis samples was mainly in the form of Cu particles. The presence of an appropriate amount of Cu particles could increase the specific surface area of Cu@Zn-NC. The subsequent batch adsorption results demonstrated that the as-fabricated composites showed high I adsorption amounts (1204.9 mg/g) and relatively fast dynamics in an iodine-cyclohexane solution when the Cu content was 30% and the pyrolysis temperature was 600 °C, outperforming the other Cu-based materials. The isothermal adsorption followed both Langmuir and Dubinin-Radushkevich isotherm models, while the kinetics of I adsorption followed a pseudo-second-order kinetic model. The activation energy () of the adsorbent was determined to be 47.2 kJ/mol, according to the Arrhenius equation. According to the experimental and DFT analyses, I-Zn interactions and I-Cu chemisorption jointly promoted the elimination of iodine. In general, this study provided an operative adsorbent for the highly effective capture of iodine in solution, which might be worth applying on a large scale.

摘要

开发高效低成本的铜基材料用于碘(I)修复是很有必要的。在此,通过球磨和热解工艺合成了铜纳米颗粒功能化的、ZIF-8(沸石咪唑框架-8)衍生的氮掺杂碳复合材料(Cu@Zn-NC)。使用扫描电子显微镜(SEM)、比表面积分析仪(BET)、X射线衍射仪(XRD)、X射线光电子能谱仪(XPS)和傅里叶变换红外光谱仪(FT-IR)对所制备的复合材料进行了表征。结果表明,引入铜盐并碳化后,ZIF-8的形态从叶状结构变为不规则结构。热解样品中的铜主要以铜颗粒的形式存在。适量铜颗粒的存在可以增加Cu@Zn-NC的比表面积。随后的批量吸附结果表明,当铜含量为30%且热解温度为600℃时,所制备的复合材料在碘-环己烷溶液中表现出高碘吸附量(1204.9 mg/g)和相对较快的动力学,优于其他铜基材料。等温吸附遵循朗缪尔和杜宾宁-拉杜什凯维奇等温线模型,而碘吸附动力学遵循准二级动力学模型。根据阿伦尼乌斯方程,确定吸附剂的活化能()为47.2 kJ/mol。根据实验和密度泛函理论(DFT)分析,I-Zn相互作用和I-Cu化学吸附共同促进了碘的去除。总的来说,本研究提供了一种用于高效捕获溶液中碘值得大规模应用的有效吸附剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4c91/11767381/feb7ad8c47da/nanomaterials-15-00105-g001.jpg

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