Wang Lei, Zhao Xinhua, Zhang Jinmiao, Xiong Zhenhu
School of Environmental Science and Engineering, Tianjin University, Tianjin, 300072, China.
School of Environmental and Municipal Engineering, Tianjin Chengjian University, Tianjin, 300384, China.
Environ Sci Pollut Res Int. 2017 Jun;24(16):14198-14206. doi: 10.1007/s11356-017-9002-9. Epub 2017 Apr 18.
Two series of metal-organic frameworks (MOFs) with similar formula units but different central metal ions (M) or organic linkers (L), M-BDC (BDC = terephthalate, M = Zn, Zr, Cr, or Fe), or Zn-L (L = imidazolate-2-methyl, BDC, BDC-NH), were prepared and employed as the receptors for adsorption lead ions. It was found that the Zn-BDC exhibited a much higher adsorption capacity than the other M-BDC series with various metal ions which have very closely low capacities at same conditions. Furthermore, the Zn-L (L = imidazolate-2-methyl, BDC, BDC-NH) still have highly efficient adsorption capacity of lead ions, although the adsorption capacity varies with different ligand, as well as the adsorption rate and the equilibrium pH of the solution. This significant high adsorption over Zn-L, different from other M-BDC series with various metal ions (Zr, Cr, or Fe), can be explained by ion exchange between the central metal ions of Zn-L and lead ion in solution. Based on the analysis of FT-IR, X-ray diffraction pattern, the nitrogen adsorption isotherms, the zeta potentials, and the results, a plausible adsorption mechanism is proposed. When equivalent Zn-L were added to equal volume of aqueous solution with different concentration of lead ion, the content of zinc ion in the solution increases with the increase of the initial concentration of lead ions. The new findings could provide a potential way to fabricate new metal organic frameworks with high and selective capacities of the heavy metal ions.
制备了两组具有相似化学式单元但中心金属离子(M)或有机连接体(L)不同的金属有机框架(MOF),即M-BDC(BDC = 对苯二甲酸酯,M = Zn、Zr、Cr或Fe)或Zn-L(L = 咪唑-2-甲基、BDC、BDC-NH),并将其用作吸附铅离子的受体。研究发现,Zn-BDC表现出比其他M-BDC系列更高的吸附容量,其他具有不同金属离子的M-BDC系列在相同条件下吸附容量非常低。此外,Zn-L(L = 咪唑-2-甲基、BDC、BDC-NH)对铅离子仍具有高效吸附容量,尽管吸附容量随不同配体以及溶液的吸附速率和平衡pH而变化。与其他具有不同金属离子(Zr、Cr或Fe)的M-BDC系列不同,Zn-L的这种显著高吸附可通过Zn-L中心金属离子与溶液中铅离子之间的离子交换来解释。基于傅里叶变换红外光谱(FT-IR)、X射线衍射图谱、氮吸附等温线、zeta电位分析及结果,提出了一种合理的吸附机制。当向等体积不同浓度铅离子的水溶液中加入等量的Zn-L时,溶液中锌离子的含量随铅离子初始浓度的增加而增加。这些新发现可为制备具有高选择性重金属离子容量的新型金属有机框架提供一条潜在途径。