Adsorptive removal of nerve-agent simulant with zirconium-based metal-organic frameworks modified by hydrophobic monocarboxylic acids

被引:23
|
作者
Cho, Kyung Ho [1 ]
Chitale, Sachin K. [2 ]
Kim, Seung-Joo [3 ,4 ]
Cha, Ga-Young [2 ]
Hong, Do-Young [1 ,2 ]
Ryu, Sam Gon [5 ]
Chang, Jong-San [1 ,6 ]
Hwang, Young Kyu [1 ,2 ]
机构
[1] KRICT, RGN, 141 Gajeong Ro, Yuseong 34114, Daejeon, South Korea
[2] UST, Dept Adv Mat & Chem Engn, 217 Gajeong Ro, Yuseong 34113, Daejeon, South Korea
[3] Ajou Univ, Dept Energy Syst Res, Suwon 16499, South Korea
[4] Ajou Univ, Dept Chem, Suwon 16499, South Korea
[5] Agcy Def Dev, POB 35-52, Yuseong 305600, Daejeon, South Korea
[6] Sungkyunkwan Univ, Dept Chem, Suwon 440476, South Korea
关键词
Toxic chemical; Zr-based metal-organic frameworks; DMMP; In situ FT-IR; DIMETHYL METHYLPHOSPHONATE DMMP; COORDINATION MODULATION; HYDROTHERMAL STABILITY; PORE-SIZE; UIO-66; DECOMPOSITION; PURIFICATION; DEGRADATION; DESTRUCTION; COMPOSITES;
D O I
10.1016/j.micromeso.2019.04.035
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
An isoreticular series of zirconium-based benzenetricarboxlyates (MOF-808) were successfully synthesized using different lengths of linear mono-carboxylic acids (i.e., formate, propionate, and valerate) as a charge-balancing ligand, and then were applied for removal of nerve-agent simulants. Removal of dimethyl methylphosphonate (DMMP) as a nerve-agent simulant of the MOF-808 analogues was conducted in dry and humid air. Tests demonstrated that the adsorption capacity of DMMP was considerably enhanced with increase in the carbon chain length of the incorporated mono-carboxylic acids of the MOF-808 (formate < propionate < valerate). The physicochemical characteristics and sorption properties of the MOF-808 analogues were thoroughly investigated using in situ FT-IR analyses and various characterization techniques, including such as XRD, N-2 sorption, TGA, SEM, Elemental Analysis (EA), and hydrophobic index (HI) measurements. It is apparent that the predominant factor affecting the MOF-808 analogues for the removal of DMMP was the concentration of surface oxygenated species (mu(3)-OH, -OH, or -OH2). These could act as active sites to adsorb DMMP via hydrogen bonding with the P=O of a DMMP molecule and then decompose it by hydrolysis. These results demonstrate that simple modulation of the surface environments of Zr-based MOFs can be adapted to tune their intrinsic efficiency for removal of toxic chemicals.
引用
收藏
页码:61 / 69
页数:9
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