CoZn-ZIF/MgAl-LDHs制备及其对碘吸附性能的研究
|
摘要
通过在双金属氢氧化物MgAl-LDHs表面定向固定纳米尺度的CoZn-ZIF,并原位生长形成CoZn-ZIF/MgAl-LDHs复合材料.利用扫描电子显微镜(SEM),傅里叶变换红外光谱仪(FT-IR),X射线衍射(XRD)和热重差热综合热分析仪(TGA/DSC)分析手段对材料进行表征,考察CoZn-ZIF/MgAl-LDHs复合材料对正己烷中碘分子的吸附行为,讨论了吸附时间和吸附温度对吸附性能的影响.此外,还对吸附过程的吸附动力学和热力学进行详细的研究,考察准一级和准二级动力学模型,Langmuir和Freundlich等温吸附模型探究该材料的吸附机理.实验结果表明,CoZn-ZIF/MgAl-LDHs对碘的吸附行为符合准二级动力学模型,吸附平衡时间为225 min.通过Langmuir等温方程得到最大平衡吸附量为344.3322 mg·g~(-1),碘的吸附过程更好地拟合Freundlich等温方程,说明反应是多分子层吸附过程,同时,由热力学数据得知该吸附是以物理吸附为主的放热过程,降低温度对吸附过程更有利.
Here, CoZn-ZIF/MgAl-LDHs was prepared through in-situ growth and CoZn-ZIF materials were directly immobilized on layered double hydroxides MgAl-LDHs. The characteristics of the materials were characterized by scanning electron microscopy(SEM), fourier transform infrared spectroscopy(FT-IR), X-ray diffraction(XRD) and thermogravimetry analysis/differential scanning calorimetry(TGA/DSC) analysis methods. To study the adsorption performance of CoZn-ZIF/MgAl-LDHs on iodine in n-hexane solution, the effect of adsorption time and temperature on adsorption performance were discussed. In addition, the adsorption kinetics and thermodynamics of the process were also studied in detail. The experimental results showed that the adsorption behavior of CoZn-ZIF/MgAl-LDHs for iodine were found to follow the pseudo-second-order kinetic model, and the adsorption equilibrium time was 225 min. The maximum equilibrium adsorption capacity was 344.3322 mg·g~(-1) by fitting the experimental data with the Langmuir isotherm equation. The adsorption process fitted the Freundlich isothermal equation better, indicating that the reaction was a multi-layer adsorption process. And it is known from the thermodynamic data that the adsorption is an exothermic process dominated by physical adsorption, adsorption capacity of iodine increased with temperature decreasing.
Here, CoZn-ZIF/MgAl-LDHs was prepared through in-situ growth and CoZn-ZIF materials were directly immobilized on layered double hydroxides MgAl-LDHs. The characteristics of the materials were characterized by scanning electron microscopy(SEM), fourier transform infrared spectroscopy(FT-IR), X-ray diffraction(XRD) and thermogravimetry analysis/differential scanning calorimetry(TGA/DSC) analysis methods. To study the adsorption performance of CoZn-ZIF/MgAl-LDHs on iodine in n-hexane solution, the effect of adsorption time and temperature on adsorption performance were discussed. In addition, the adsorption kinetics and thermodynamics of the process were also studied in detail. The experimental results showed that the adsorption behavior of CoZn-ZIF/MgAl-LDHs for iodine were found to follow the pseudo-second-order kinetic model, and the adsorption equilibrium time was 225 min. The maximum equilibrium adsorption capacity was 344.3322 mg·g~(-1) by fitting the experimental data with the Langmuir isotherm equation. The adsorption process fitted the Freundlich isothermal equation better, indicating that the reaction was a multi-layer adsorption process. And it is known from the thermodynamic data that the adsorption is an exothermic process dominated by physical adsorption, adsorption capacity of iodine increased with temperature decreasing.
引文
蔡璇, 刘燕, 张云, 等. 2012. 核事故产生的放射性废水处理方法研究进展[J]. 化学通报, (6): 483-488
陈建东, 许伟城, 吴军良, 等. 2017. 金属有机框架ZIF-8/聚二乙烯基苯纳米复合材料的合成及其吸附VOCs的性能[J]. 环境科学学报, 37(5): 1877-1883
范祎, 李成吾. 2011. 尿素水热法制备Mg/Al/Fe多元水滑石及其阻燃性能研究[J]. 有色矿冶, 27(1): 33-36
李发炎, 胡章文,刘俊. 2013. 共沉淀法制备镁铝双金属氢氧化物及表征[J]. 轻金属, (6):15-17
李小娟, 何长发, 黄斌, 等. 2016. 金属有机骨架材料吸附去除环境污染物的进展[J]. 化工进展, 35(2): 586-594
廖梅芳, 朱文杰, 韩彩芸, 等. 2016. 镁铝水滑石的制备及其吸附Cr(Ⅵ) 的性能[J]. 安全与环境学报, 16(6): 200-207
林益军, 朱云龙, 旷桂超, 等. 2017. 用于放射性碘吸附的多孔有机聚合物[J]. 化学进展, 29(7): 766-775
马玉玲, 马杰, 陈雅丽, 等. 2018. 水铁矿及其胶体对砷的吸附与吸附形态[J]. 环境科学, 39(1): 179-186
Ping L, Hua C Z. 2016. Immobilization of metal-organic framework nanocrystals for advanced design of supported nanocatalysts[J]. Acs Applied Materials & Interfaces, 8(43): 29551
祁兵兵, 茆平, 杨毅. 2016. 金属有机骨架材料MIL-101用于气态碘单质的吸附与释放[J]. 装备环境工程, 13(6): 5-9
邱健豪, 何明, 贾明民, 等. 2016. 金属有机骨架材料制备双金属或多金属催化材料及其应用[J]. 化学进展, 28(7): 1016-1028
王奖, 徐爱菊, 贾美林, 等. 2017. Mg-Al类水滑石负载金催化醇选择氧化中Mg/Al比例的影响[J]. 分子催化, 31(1): 11-21
王军锋. 2006. 纳米Mg/Al-LDH制备工艺研究及结构表征[D]. 西安:西安理工大学
王龙江, 马英, 俞杰, 等. 2017. 金属有机骨架材料捕集气态放射性碘的研究进展[J]. 现代化工, 37(9): 62-65
Xue X, Zhang H, Zhang S. 2014. Preparation of MgAl LDHs Intercalated with Amines and Effect on Thermal Behavior for Poly(vinyl chloride)[J]. Advances in Materials Physics & Chemistry, 4(12): 258-266
Yang J, Zhang F J, Lu H Y, et al. 2015. Hollow Zn/Co ZIF particles derived from core-shell ZIF-67@ZIF-8 as selective catalyst for the semi-hydrogenation of acetylene[J]. Angewandte Chemie, 127(37): 11039-11043
张贺, 李国良, 张可刚, 等. 2017. 金属有机骨架材料在吸附分离研究中的应用进展[J]. 化学学报, 75(9): 841-859
张树芹, 侯万国, 路福绥, 等. 2010. MgAl无机-有机杂化材料对Pb2+的吸附[J]. 应用化学, 27(2): 142-146
周玉晓. 2016. 金属有机骨架材料及其衍生物在多相催化中的应用[D]. 合肥:中国科学技术大学
曾艾群. 2016. 金属有机骨架(MOFs)作为电极材料在二次锂离子电池中的应用[J]. 电子世界, (17): 200-201
朱清, 李成胜, 周建成. 2017. 镁铝水滑石的共沉淀法制备及表征[J]. 化工时刊, 31(4): 1-3+17
陈建东, 许伟城, 吴军良, 等. 2017. 金属有机框架ZIF-8/聚二乙烯基苯纳米复合材料的合成及其吸附VOCs的性能[J]. 环境科学学报, 37(5): 1877-1883
范祎, 李成吾. 2011. 尿素水热法制备Mg/Al/Fe多元水滑石及其阻燃性能研究[J]. 有色矿冶, 27(1): 33-36
李发炎, 胡章文,刘俊. 2013. 共沉淀法制备镁铝双金属氢氧化物及表征[J]. 轻金属, (6):15-17
李小娟, 何长发, 黄斌, 等. 2016. 金属有机骨架材料吸附去除环境污染物的进展[J]. 化工进展, 35(2): 586-594
廖梅芳, 朱文杰, 韩彩芸, 等. 2016. 镁铝水滑石的制备及其吸附Cr(Ⅵ) 的性能[J]. 安全与环境学报, 16(6): 200-207
林益军, 朱云龙, 旷桂超, 等. 2017. 用于放射性碘吸附的多孔有机聚合物[J]. 化学进展, 29(7): 766-775
马玉玲, 马杰, 陈雅丽, 等. 2018. 水铁矿及其胶体对砷的吸附与吸附形态[J]. 环境科学, 39(1): 179-186
Ping L, Hua C Z. 2016. Immobilization of metal-organic framework nanocrystals for advanced design of supported nanocatalysts[J]. Acs Applied Materials & Interfaces, 8(43): 29551
祁兵兵, 茆平, 杨毅. 2016. 金属有机骨架材料MIL-101用于气态碘单质的吸附与释放[J]. 装备环境工程, 13(6): 5-9
邱健豪, 何明, 贾明民, 等. 2016. 金属有机骨架材料制备双金属或多金属催化材料及其应用[J]. 化学进展, 28(7): 1016-1028
王奖, 徐爱菊, 贾美林, 等. 2017. Mg-Al类水滑石负载金催化醇选择氧化中Mg/Al比例的影响[J]. 分子催化, 31(1): 11-21
王军锋. 2006. 纳米Mg/Al-LDH制备工艺研究及结构表征[D]. 西安:西安理工大学
王龙江, 马英, 俞杰, 等. 2017. 金属有机骨架材料捕集气态放射性碘的研究进展[J]. 现代化工, 37(9): 62-65
Xue X, Zhang H, Zhang S. 2014. Preparation of MgAl LDHs Intercalated with Amines and Effect on Thermal Behavior for Poly(vinyl chloride)[J]. Advances in Materials Physics & Chemistry, 4(12): 258-266
Yang J, Zhang F J, Lu H Y, et al. 2015. Hollow Zn/Co ZIF particles derived from core-shell ZIF-67@ZIF-8 as selective catalyst for the semi-hydrogenation of acetylene[J]. Angewandte Chemie, 127(37): 11039-11043
张贺, 李国良, 张可刚, 等. 2017. 金属有机骨架材料在吸附分离研究中的应用进展[J]. 化学学报, 75(9): 841-859
张树芹, 侯万国, 路福绥, 等. 2010. MgAl无机-有机杂化材料对Pb2+的吸附[J]. 应用化学, 27(2): 142-146
周玉晓. 2016. 金属有机骨架材料及其衍生物在多相催化中的应用[D]. 合肥:中国科学技术大学
曾艾群. 2016. 金属有机骨架(MOFs)作为电极材料在二次锂离子电池中的应用[J]. 电子世界, (17): 200-201
朱清, 李成胜, 周建成. 2017. 镁铝水滑石的共沉淀法制备及表征[J]. 化工时刊, 31(4): 1-3+17