School of Chemistry and Chemical Engineering, Institute for Smart Materials and Engineering, University of Jinan, Jinan 250022, PR China; School of Pharmaceutical Sciences & Institute of Materia Medica, Shandong First Medical University & Shandong Academy of Medical Sciences, Jinan 250117, PR China.
School of Chemistry and Chemical Engineering, Institute for Smart Materials and Engineering, University of Jinan, Jinan 250022, PR China.
Int J Biol Macromol. 2023 Dec 31;253(Pt 7):127110. doi: 10.1016/j.ijbiomac.2023.127110. Epub 2023 Sep 30.
Current cellulose-based adsorbents suffer from the drawbacks of low adsorption capacity or slow adsorption rate for heavy metal ions. It is imperative to prepare new cellulose-based materials to improve the adsorption ability. In this work, we aim to introduce phosphonate groups to improve the adsorption ability of cellulose and select polyethyleneimine (PEI) for synergistic adsorption. A novel cellulose phosphonate/polyethyleneimine composite (MCCP-PEI) is prepared via the Mannich reaction. The structure and composition of MCCP-PEI are characterized by various advanced microscopy and spectroscopy techniques, and the results show that MCCP-PEI possesses abundant nano-porous structure, strong chelating sites, and excellent hydrophilicity. Besides, the adsorption behavior of MCCP-PEI for heavy metals has been systematically investigated. The results show that the adsorbent can quickly remove toxic Cu(II) and Pb(II) from water within 15 min and 20 min, respectively. The saturated adsorption capacity for Cu(II) and Pb(II) is 250.0 and 534.7 mg·g, respectively. X-ray photoelectron spectroscopy analysis combined with Density Functional Theory calculations reveal that the adsorption mechanism is chemical complexation and electrostatic attraction, and the phosphonate group plays a key role in the adsorption process.
目前基于纤维素的吸附剂存在重金属离子吸附容量低或吸附速率慢的缺点。因此，迫切需要制备新型纤维素基材料以提高吸附能力。在这项工作中，我们旨在引入膦酸基团来提高纤维素的吸附能力，并选择聚乙烯亚胺（PEI）进行协同吸附。通过曼尼希反应制备了一种新型纤维素磷酸酯/聚乙烯亚胺复合材料（MCCP-PEI）。采用各种先进的显微镜和光谱技术对 MCCP-PEI 的结构和组成进行了表征，结果表明 MCCP-PEI 具有丰富的纳米多孔结构、强螯合位点和优异的亲水性。此外，还系统研究了 MCCP-PEI 对重金属的吸附行为。结果表明，该吸附剂能够在 15 分钟和 20 分钟内快速去除水中的有毒 Cu(II)和 Pb(II)。Cu(II)和 Pb(II)的饱和吸附容量分别为 250.0 和 534.7 mg·g。X 射线光电子能谱分析结合密度泛函理论计算表明，吸附机制是化学络合和静电吸引，膦酸基团在吸附过程中起关键作用。
