三取代 4f 和 4d 钨锑酸盐作为神经毒剂降解的人工磷酸酯酶。
Trisubstituted 4f- and 4d tungstoantimonates as artificial phosphoesterases for nerve agent degradation.
机构信息
Universität Wien, Fakultät für Chemie, Institut für Biophysikalische Chemie, 1090 Wien, Austria.
出版信息
Chem Commun (Camb). 2022 Jul 12;58(56):7761-7764. doi: 10.1039/d2cc02223k.
Three new trisubstituted 4f- and 4d tungstoantimonates (TA) KNa[(M(CHCOO))(HPO)(WO)(SbWO)]·HO {M3(HPO3)Sb3W28} (M = Gd, Y, Yb, = 35-36) were synthesized using a double-template synthetic approach. Following their characterization in the solid state employing single- and powder X-ray diffraction (XRD), IR-spectroscopy, and elemental - and thermogravimetric analyses (TGA), {M3(HPO3)Sb3W28} were subjected to a comprehensive set of solution characterization methods including UV/vis- and multinuclear P and C NMR spectroscopy. All representatives were shown to be highly active, recyclable, and stable Lewis-acid catalysts towards the nerve agent simulant ,-dimethyl -(4-nitrophenyl) phosphate (DMNP) at neutral pH (in Tris-HCl [125 mM] at pD 7.0 25 °C). Control experiments showing catalytic activity of the unsubstituted trilacunary [SbWO] suggest the non-innocence of Tris in the DMNP hydrolysis for the first time.
使用双模板合成方法合成了三种新的三取代 4f 和 4d 钨锑酸盐（TA）KNa[(M(CHCOO))(HPO)(WO)(SbWO)]·HO {M3(HPO3)Sb3W28}（M = Gd、Y、Yb， = 35-36）。通过单晶和粉末 X 射线衍射（XRD）、红外光谱、元素和热重分析（TGA）对其在固态下的特性进行了表征，然后对 {M3(HPO3)Sb3W28} 进行了一系列全面的溶液特性分析方法，包括 UV/vis 和多核 P 和 C NMR 光谱。所有代表物在中性 pH（25°C 时 Tris-HCl [125 mM] 中的 pD 7.0）下对神经毒剂模拟物 -二甲基-（4-硝基苯基）磷酸酯（DMNP）均表现出高活性、可回收和稳定的路易斯酸催化剂性能。首次控制实验表明，未取代的三齿 [SbWO] 具有催化活性，这表明 Tris 在 DMNP 水解中并非无活性。
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