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文章以杨树木粉为骨架，通过碱预处理与多胺试剂进行反应，合成了4种不同胺基链长的多胺木粉(AWFs)，并考察其对常见畜禽废水中4种药源有机物的去除性能。结果表明，AWFs对磺胺甲恶唑(SMZ)、头孢唑林(CEF)、对氨基苯砷酸(p-ASA)和对苯二酚(HQ)的最优pH均接近其酸性基团的p Ka值，总体上随多胺链长增大先增后降，三乙烯四胺改性木粉(TTWF)吸附量最大。将其与聚胺改性木粉(PWF)对比研究，4种污染物在TTWF和PWF上的吸附均符合Langmuir模型，TTWF和PWF分别对HQ和SMZ的饱和吸附量最大，为3.877 mmol/g和2.432 mmol/g。此外，TTWF和PWF对SMZ、CEF和p-ASA的吸附随温度变化影响是相反的，可能是由于前者对这些药源有机物的吸附以氢键作用为主导，是自发的吸热反应，而后者的多胺基碱性强，以静电吸附为主。采用密度泛函理论(DFT)优化计算了它们与TTWF的静电和氢键作用构型，总结合能顺序与吸附容量的排序一致。
Abstract：Poplar wood powder was used as the matrix for alkali pretreatment and subsequent reaction with polyamine reagents to synthesize four types of polyamine-modified wood powders(AWFs) with different amino chain lengths. The removal performance of these AWFs for four medicinal-origin organics in livestock wastewater was investigated. The optimal p H values for the adsorption of sulfamethazine(SMZ), cefotaxime(CEF), p-arsanilic acid(p-ASA), and hydroquinone(HQ) onto different AWFs are all close to the p Ka values of their acidic groups. Generally, the adsorption capacity initially increases and then decreases with the increase in polyamine chain length, with triethylene tetraminemodified wood powder(TTWF) exhibiting the highest adsorption capacity. A comparative study with polyaminemodified wood powder(PWF) reveals that the adsorption of the four pollutants on TTWF and PWF fitted better with the Langmuir isotherm model. The adsorption capacities of HQ on TTWF and SMZ on PWF are the highest among the four adsorbates, which are 3.877 and 2.432 mmol/g, respectively. Additionally, the adsorption of SMZ, CEF, and p-ASA on TTWF and PWF exhibits opposite temperature dependencies, possibly due to the dominant hydrogen bonding interaction for the former, leading to an endothermic spontaneous adsorption reaction, while the latter, with stronger alkalinity of polyamine groups, primarily involves electrostatic adsorption. Density functional theory(DFT) optimization calculations are employed to analyze the electrostatic and hydrogen bonding interactions between the drugs and TTWF, and the order of total binding energies is well consistent with the adsorption capacity ranking.
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基本信息:
DOI：10.16026/j.cnki.iea.2024050404
中图分类号:X713;O647.3
引用信息:
[1]黄子懿,陈婕妤,宋逸璇等.多胺改性木粉对水体中药源有机物的吸附对比研究[J].离子交换与吸附,2024,40(05):404-411.DOI:10.16026/j.cnki.iea.2024050404.
基金信息:
国家自然科学基金(基金号51708281); 大学生实践创新训练计划项目(项目号2022NJFUSPITP0371)