发色团官能化的锆MOF对神经毒剂VX的降解和检测,Chemistry of Materials

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发色团官能化的锆MOF对神经毒剂VX的降解和检测
Chemistry of Materials ( IF 7.2 ) Pub Date : 2019-08-21 00:00:00 , DOI: 10.1021/acs.chemmater.9b02073
Martijn C. de Koning ₁ , Gregory W. Peterson ₂ , Marco van Grol ₁ , Ivan Iordanov ₂ , Monica McEntee ₂

Affiliation

神经制剂是人类已知的最剧毒的物质。叙利亚，马来西亚和英国最近发生的事件表明，这些物质的威胁是真实存在的。及时检测和鉴定神经毒剂对于促进及时去污或医疗对策非常重要。在这项工作中，开发了一种基于金属-有机框架（MOF）NU-1000的有效而灵敏的检测系统，用于公开V剂，V剂是一种非常持久，剧毒且困难的神经剂。检测。NU-1000是基于锆的MOF，可以将VX水解为无毒的膦酸和硫醇2-（二异丙基氨基）乙硫醇。在这项工作中，假设该MOF的每块Zr合成砖上存在的四个非配位位点都可以用DTNB的5,5'-二硫代-双（2-硝基苯甲酸）中存在的两个羧酸酯官能化。这种二聚体（RS-SR）化合物通过S-S键交换与硫醇有效反应，并导致发色团RS-H释放。因此，预期目标杂化材料（DTNB @ NU-1000）降解VX，同时在VX的含硫醇降解产物与MOF结合的DTNB反应时产生可见的颜色响应。我们在这里报告DTNB @ NU-1000可以很容易地合成，并且在中性缓冲液中VX的降解中具有令人惊讶的活性。此外，VX的降解导致颜色响应，其强度与所使用的VX浓度呈线性关系。该材料的适用性通过针对VX污染的表面的概念验证检测套件进行了说明，例如涂有VX污染的金属板（涂有军用漆[耐化学试剂的涂层]）。此过程需要最少的培训负担，并且VX污染低至约1-2μg/ cm在20分钟的总处理时间内，可以可靠地从视觉上确定²。

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Degradation and Detection of the Nerve Agent VX by a Chromophore-Functionalized Zirconium MOF

Nerve agents are among the most toxic substances known to man. Recent events in Syria, Malaysia, and the UK illustrate that the threat of these substances is real and actual. The timely detection and identification of nerve agents is of great importance to facilitate timely decontamination or medical countermeasures. In this work, an effective and sensitive detection system, based on the metal–organic framework (MOF) NU-1000, was developed for the disclosure of V-agents, a class of nerve agents that is very persistent, highly toxic, and difficult to detect. NU-1000 is a zirconium-based MOF that can hydrolyze VX into a nontoxic phosphonic acid and the thiol 2-(diisopropylamino)ethanethiol. In this work, it was hypothesized that the four noncoordinating sites that are present on each Zr-building brick of this MOF could be functionalized with the two carboxylates present in 5,5′-di-thio-bis(2-nitrobenzoic acid), DTNB. This dimeric (RS-SR) compound efficiently reacts with thiols by S–S bond exchange and results in the release of the chromophore RS-H. Thus, the target hybrid material (DTNB@NU-1000) was expected to degrade VX and at the same time give a visual color response upon reaction of the thiol-containing degradation product of VX with MOF-bound DTNB. We here report that DTNB@NU-1000 can be readily synthesized and that it is surprisingly active in the degradation of VX in neutral buffer. Moreover, the degradation of VX resulted in a color response, the intensity of which showed linear correlation with the VX concentration used. The applicability of this material was illustrated by a proof-of-concept detection kit for VX-contaminated surfaces, as exemplified with VX-contaminated metal panels coated with military paint [chemical agent resistant coating]. This procedure requires minimal training burden, and VX contamination down to a level of about 1–2 μg/cm² could be reliably visually established, during a total handling time of 20 min.

更新日期：2019-08-21

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