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Mixed-Metal Cerium/Zirconium MOFs with Improved Nerve Agent Detoxification Properties
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-11-05 , DOI: 10.1021/acs.inorgchem.0c01434
Elham Geravand 1 , Faezeh Farzaneh 1 , Rodrigo Gil-San-Millan 2 , Francisco J. Carmona 2 , Jorge A. R. Navarro 2
Affiliation  

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)2 doping of the mixed-metal MOFs as exemplified with M01@Mg(OMe)2 and M02@Mg(OMe)2 systems. The results show that Mg(OMe)2 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)2 1:2 and M02@Mg(OMe)2 1:4, respectively.

中文翻译:

具有改善的神经毒剂解毒性能的混合金属铈/锆MOF

一系列具有不同拓扑/连接性的Ce / Zr混合金属有机框架,即Ce / Zr-UiO-66(U01,U02和U03)(fcu(12-c)),Ce / Zr-DUT-对67-PZDC(D01和D02)(reo(8-c))和Ce / Zr-MOF-808(M01,M02和M03)(spn(6-c))进行了毒性神经毒剂排毒评估室温下在无缓冲水溶液中的二异丙基氟磷酸二异丙酯(DIFP)模型。值得注意的是,PF键断裂的催化速率随Ce / Zr摩尔比的增加而增加。如M01 @ Mg(OMe)2和M02 @ Mg(OMe)2系统所示,混合金属MOF的Mg(OMe)2掺杂可以实现催化活性的进一步提高。结果表明,Mg(OMe)2M01 @ Mg(OMe)2 1:2和M02掺入M01和M02的介孔腔中会导致P–F水解降解半衰期将近5和2分钟,而DIFP会100%降解。@Mg(OMe)2分别为1:4。
更新日期:2020-11-05
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