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
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
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DOI：
10.1021/acs.inorgchem.7b01809
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发表时间：
2017-10-02
影响因子：
4.6
通讯作者：
Breijaert, Troy
中科院分区：
文献类型：
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作者：
de Koning, Martijn C.;van Grol, Marco;Breijaert, Troy
近年来，已经开发了基于Zr的金属有机框架（M0 F），其促进有毒有机磷酸酯试剂（例如化学战剂（CWA））的催化降解。由于严格的规定，大多数实验室不可能使用活体试剂进行实验，因此在大多数情况下使用模拟物。使用真实的化学武器的报告很少，而且没有涵盖所有的化学武器。我们在这里提出了一个比较研究，其中UIO-66-NH 2，NU-1000，MOF-808，PCN-777的降解对氧磷和化学战剂塔崩，VX，梭曼，在N-乙基吗啉缓冲液（pH 10）以及在纯水中的有效性进行了评估。所有MOFs在碱性条件下均表现出优异的降解能力。进一步揭示了塔崩根据条件通过不同的机制降解。胺的存在，无论是作为MOF结构的一部分（U10 -66-NH 2）或在代理本身（VX，塔崩），是最重要的因素，在水中的降解速率。结果表明，MOFs在未来的防护应用中具有很大的潜力。虽然模拟物的使用为新的MOFs的初步筛选和选择提供了有价值的信息，但活性剂的使用揭示了额外的机制，这将有助于未来开发更好的催化剂。
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.