多基团秸秆纤维对水体中铜/磺胺甲恶唑复合污染物的定量吸附性能  

Quantitative adsorption behavior of copper/sulfonamides compound pollutants in aqueous solution by multi-groups straw fibers

作　　者：孟佩佩 张丹凤 伦乐豪 苏耀明 张娜 周倩雅 章莉娟[4] 郑刘春[2,5,6] MENG Peipei;ZHANG Danfeng;LUN Lehao;SU Yaoming;ZHANG Na;ZHOU Qianya;ZHANG Lijuan;ZHENG Liuchun(College of Environment,Jinan University,Guangzhou 511436,China;School of Environment,South China Normal University,Guangzhou 510006,China;South China Institute of Environmental Sciences,Guangzhou 510655,China;School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510640,China;Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety,Guangzhou 510006,China;MOE Key Laboratory of Theoretical Chemistry of Environment,Guangzhou 510006,China)

机构地区：[1]暨南大学环境学院,广州511436 [2]华南师范大学环境学院,广州510006 [3]生态环境部华南环境科学研究所,广州510655 [4]华南理工大学,化学与化工学院,广州510640 [5]华南师范大学,广东省化学品污染与环境安全重点实验室,广州510006 [6]华南师范大学,教育部环境理论化学重点实验室,广州510006

出　　处：《环境工程学报》2023年第2期390-403,共14页Chinese Journal of Environmental Engineering

基　　金：国家自然科学基金(52170035);广东省重点领域研发计划项目(2019B110207001);中央级公益性科研院所基本科研业务专项(PM-zx703-201803-069);广州市民生科技攻关计划项目(201803030001)。

摘　　要：以秸秆纤维为研究对象,通过醚化和接枝化修饰方法赋予其纤维结构的季胺基(-N+)、羧基(-COOH)等,从而制备出多基团纤维材料(NCS)。在一元和二元吸附体系中,考察了NCS对不同pH水体中铜/磺胺甲恶唑(SMZ-Cu)复合污染物的去除效果。Langmuir吸附等温线拟合结果表明,NCS对SMZ和Cu(Ⅱ)的最大理论吸附量分别为59.76 mg·g^(-1)和4.71 mg·g^(-1),以及对络合物中SMZ和Cu(Ⅱ)的最大理论吸附量分别为56.21 mg·g^(-1)和5.54 mg·g^(-1)。吸附过程也符合准二级动力学方程,属于化学吸附。相比而言,NCS在一元吸附体系中更倾向单一吸附SMZ而不是Cu(Ⅱ)。而且,多重相互作用使NCS在二元吸附体系中主要吸附SMZ-Cu为主,而不是单一污染物。密度泛函理论(DFT)计算不但验证了上述结果,还定量地解释在单一吸附系统中,NCS的-N+结构中-COOH与SMZ中磺酰氨氮结合最稳定,而C-N则与Cu结合能最大;在二元吸附体系中,最主要的吸附结构是SMZ-Cu以Cu接近NCS方式,而络合-解络合-再络合模式是该体系中Cu被吸附增加的原因。Straw fiber was selected as the research object, and then multigroup fiber materials(NCS) were prepared by endowing quaternary amine groups(-N+) and carboxyl groups(-COOH) onto fiber structures through etherification and grafting modification methods. In the single and binary adsorption systems, the removal effects of NCS on copper/sulfamethoxazole(SMZ-Cu) combined pollutants in water at different pHs were investigated. The fitting results of Langmuir adsorption isotherms showed that the maximum theoretical adsorption capacities of NCS to SMZ and Cu(Ⅱ) were 59.76 mg·g^(-1)and 4.71 mg·g^(-1), respectively, and the maximum theoretical adsorption capacities of SMZ and Cu(Ⅱ) in the complex were 56.21 mg·g^(-1)and 5.54 mg·g^(-1), respectively. The adsorption process also conformed to the pseudo-second-order kinetic equation,and belonged to chemical adsorption. In contrast, NCS was more likely to adsorb SMZ than Cu(Ⅱ) in the single system. Moreover, the multiple interactions caused NCS to mainly adsorb SMZ-Cu in the binary system rather than a single pollutant. Density functional theory(DFT) calculations not only verified the above analysis, but also quantitatively explained the following results in the single adsorption system: In the-N+structure of NCS,-COOH had the most stable binding energy with sulfonamide nitrogen in SMZ, while C-N had the largest binding energy with Cu. In the binary adsorption system, the most dominant adsorption mechanism was that SMZ-Cu approached NCS in the form of Cu, and the complexation–decomplexation–complexation mode was the reason for increasing Cu adsorption.

关 键 词：秸秆纤维 铜/磺胺类抗生素复合物 基团 吸附行为 定量计算 

分 类 号：X703[环境科学与工程—环境工程]