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Degradation of Paraoxon and the Chemical Warfare Agents VX, Tabun, and Soman by the Metal–Organic Frameworks UiO-66-NH2, MOF-808, NU-1000, and PCN-777
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2017-09-19 00:00:00 , DOI: 10.1021/acs.inorgchem.7b01809
Martijn C. de Koning 1 , Marco van Grol 1 , Troy Breijaert 1
Affiliation  

In recent years, Zr-based metal–organic frameworks (MOFs) have been developed that facilitate catalytic degradation of toxic organophosphate agents, such as chemical warfare agents (CWAs). Because of strict regulations, experiments using live agents are not possible for most laboratories and, as a result, simulants are used in the majority of cases. Reports that employ real CWAs are scarce and do not cover the whole spectrum of agents. We here present a comparative study in which UiO-66-NH2, NU-1000, MOF-808, and PCN-777 are evaluated for their effectiveness in the degradation of paraoxon and the chemical warfare agents tabun, VX, and soman, in N-ethylmorpholine buffer (pH 10) as well as in pure water. All MOFs showed excellent ability to degrade the agents under basic conditions. It was further disclosed that tabun is degraded by different mechanisms depending on the conditions. The presence of an amine, either as part of the MOF structure (UiO-66-NH2) or in the agent itself (VX, tabun), is the most important factor governing degradation rates in water. The results show that MOFs have great potential in future protective applications. Although the use of simulants provides valuable information for initial screening and selection of new MOFs, the use of live agents revealed additional mechanisms that should aid the future development of even better catalysts.

中文翻译:

金属有机骨架UiO-66-NH 2,MOF-808,NU-1000和PCN-777降解对氧磷和化学战剂VX,塔邦和索曼

近年来,已经开发出基于Zr的金属有机框架(MOF),以促进有毒有机磷酸盐试剂(例如化学战剂(CWA))的催化降解。由于严格的规定,大多数实验室无法使用活性剂进行实验,因此,大多数情况下都使用了模拟物。使用实际CWA的报告很少,并且不能涵盖代理商的全部范围。我们在这里提供了一项比较研究,其中评估了UiO-66-NH 2,NU-1000,MOF-808和PCN-777在对氧磷和化学战剂塔邦,VX和梭曼的降解中的有效性。ñ-乙基吗啉缓冲液(pH 10)以及在纯水中。在基本条件下,所有MOF均具有出色的降解试剂的能力。进一步公开了取决于条件,塔宾通过不同的机制降解。作为MOF结构的一部分(UiO-66-NH 2)或在试剂本身(VX,tabun)中,胺的存在是控制水中降解速率的最重要因素。结果表明,MOF在未来的防护应用中具有巨大的潜力。尽管使用模拟物为新的MOF的初步筛选和选择提供了有价值的信息,但使用活性剂揭示了更多的机制,这些机制应有助于未来更好的催化剂的开发。
更新日期:2017-09-19
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