Department of Chemistry, Faculty of Physics and Chemistry, Alzahra University, Vanak, Tehran 19938 91176, Iran.
Departamento de Química Inorgánica, Universidad de Granada, Avenida Fuentenueva S/N, 18071 Granada, Spain.
Inorg Chem. 2020 Nov 16;59(22):16160-16167. doi: 10.1021/acs.inorgchem.0c01434. Epub 2020 Nov 5.
A series of Ce/Zr mixed-metal-organic frameworks with different topology/connectivity, namely, Ce/Zr-UiO-66 (U01, U02, and U03) (fcu (12-c)), Ce/Zr-DUT-67-PZDC (D01 and D02) (reo (8-c)), and Ce/Zr-MOF-808 (M01, M02, and M03) (spn (6-c)) were evaluated toward the detoxification of toxic nerve agent model diisopropylfluorophosphate (DIFP) at room temperature in unbuffered aqueous solution. Noteworthily, the catalytic rate for P-F bond cleavage increased with increasing Ce/Zr molar ratio. A further increase in catalytic activity can be achieved by Mg(OMe) doping of the mixed-metal MOFs as exemplified with M01@Mg(OMe) and M02@Mg(OMe) systems. The results show that Mg(OMe) incorporation into the mesoporous cavities of M01 and M02 give rise to P-F hydrolytic degradation half-lives of nearly 5 and 2 min with 100% degradation of DIFP after 55 and 65 min for M01@Mg(OMe) 1:2 and M02@Mg(OMe) 1:4, respectively.
一系列具有不同拓扑/连接性的 Ce/Zr 混合金属有机骨架，即 Ce/Zr-UiO-66（U01、U02 和 U03）（fcu（12-c））、Ce/Zr-DUT-67-PZDC（D01 和 D02）（reo（8-c））和 Ce/Zr-MOF-808（M01、M02 和 M03）（spn（6-c）），在无缓冲水溶液中于室温下对有毒神经毒剂模型二异丙基氟磷酸（DIFP）的解毒作用进行了评估。值得注意的是，P-F 键断裂的催化速率随 Ce/Zr 摩尔比的增加而增加。通过将混合金属 MOFs 中的 Mg(OMe) 掺杂，可以进一步提高催化活性，例如 M01@Mg(OMe) 和 M02@Mg(OMe) 体系。结果表明，Mg(OMe) 掺入 M01 和 M02 的介孔腔中，导致 P-F 水解降解半衰期分别接近 5 和 2 min，并且在 55 和 65 min 后，DIFP 的降解率达到 100%，对于 M01@Mg(OMe) 1:2 和 M02@Mg(OMe) 1:4 分别为。
