阳离子化柱[5]芳烃改性沸石对溴甲酚紫的吸附研究  

Preparation of Cationic Water-Pillar [5] arene Modified Zeolite and Its Adsorption to Bromocresol Purple

作　　者：杨云汉 杨俊丽 鲁佳佳 李灿花 古捷 陈文[2] 杨丽娟 YANG Yun-Han;YANG Jun-Li;LU Jia-Jia;LI Can-Hua;GU Jie;CHEN Wen;YANG Li-Juan(Key Laboratory of Intelligent Supramolecular Chemistry at the University of Yunnan Province,National and Local Joint Engineering Research Center for Green Preparation Technology of Biobased Materials,School of Chemistry&Environment,Yunnan Minzu University,Kunming 650500,China;Key Laboratory of Medicinal Chemistry for Natural Resources,Ministry of Education,School of Chemical Science and Technology,Yunnan University,Kunming 650091,China)

机构地区：[1]云南民族大学化学与环境学院云南省高校智能超分子化学重点实验室生物基材料绿色制备技术国家地方联合工程中心,昆明650500 [2]云南大学教育部自然资源药物化学重点实验室,昆明650091

出　　处：《分析化学》2019年第12期1922-1930,共9页Chinese Journal of Analytical Chemistry

基　　金：国家自然科学基金项目(Nos.21562048,21762051);云南省高校有机功能分子及材料科技创新团队项目;云南省教育厅科学研究基金项目(No.2019Y0193)资助~~

摘　　要：制备了阳离子化柱[5]芳烃改性沸石(CP5A/NZ),采用扫描电镜(SEM)、红外吸收光谱(IR)和X-射线粉末衍射(XRD)对CP5A/NZ进行表征,将其应用于阴离子染料溴甲酚紫(BCP)的吸附。考察了NZ粒径、改性时CP5A的浓度、吸附时间、BCP初始浓度和溶液pH值对BCP清除率的影响,分析了CP5A/NZ吸附BCP的动力学过程和吸附等温线,探讨了其吸附机制。SEM表征结果表明,经CP5A改性后,NZ具有的鳞片状结构消失,呈现体积增大的包块状结构;IR谱图中可以观察到CP5A/NZ中出现了CP5A中CH3N+和CH2N+的振动吸收峰;XRD揭示了NZ经CP5A改性后具有不同的晶体结构,上述结果均表明CP5A成功负载到NZ上。吸附研究结果表明,由于电荷斥力,NZ对BCP没有清除能力,但使用10 g/L的CP5A溶液改性粒径为0.42~0.59 nm的NZ时,其对BCP的清除率达94.0%,且吸附在300 min时达到平衡,而CP5A/NZ处理低浓度(<100 mg/L)BCP溶液时具有较高的清除率。二级动力学方程和Langmuir型等温线能更好地描述CP5A/NZ对BCP的吸附过程。推测CP5A/NZ对BCP的吸附机理为:CP5A中的CH2N+与NZ发生阳离子交换后, CH2N+与NZ表面的负电位点结合,使NZ表面的正电荷活性吸附位点增加,从而对阴离子染料BCP具有较好的清除能力。The cationic water-pillar[5]arene(CP5 A) modified zeolite(NZ) was prepared for adsorption of anionic dye bromocresol purple(BCP). The CP5 A/NZ was characterized by scanning electron microscopy(SEM), infrared absorption spectroscopy(IR) and X-ray powder diffraction(XRD). The effects of NZ particle size, concentration of CP5 A during modification, adsorption time, initial BCP concentration and solution pH on the removal percentage of BCP were studied. In addition, the kinetics and adsorption isotherms of BCP adsorption by CP5 A/NZ were also analyzed, and the adsorption mechanism was discussed. SEM showed that the scaly structure of the NZ disappeared after CP5 A modification, showing an enlarged bulk structure. The vibration of CH3N+ and CH2N+ in CP5 A appeared in the CP5 A/NZ. XRD revealed that the zeolite had different crystal structure after CP5 A modification, and all of the above phenomena indicated that CP5 A was successfully loaded into the NZ. Adsorption studies showed that due to charge repulsion, NZ had no scavenging ability to BCP. However, when CP5 A solution(10 g/L) was used to modify NZ in the range of 0.42-0.59 nm, the removal percentage of BCP was 93.98%, and the adsorption reached equilibrium in 300 min. CP5 A/NZ had a high removal percentage when treated with low concentrations(< 100 mg/L) of BCP solution. The second-order kinetic equation and the Langmuir isotherm could better fit the adsorption process of CP5 A/NZ to BCP. The adsorption mechanism of CP5 A/NZ on BCP could be described as follows: after the cation exchange of CH2N+ with NZ in CP5 A, CH2N+ bound to the negative potential point on the surface of NZ, which increased the positive charge activity adsorption site of NZ surface, and thus the anion dye BCP had good scavenging ability.

关 键 词：沸石 芳烃 溴甲酚紫 改性 吸附 

分 类 号：X70[环境科学与工程—环境工程]