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Zn(II)-alloferon complexes – Similar sequence, different coordination modes, no antibacterial activity
Journal of Inorganic Biochemistry ( IF 3.9 ) Pub Date : 2020-10-13 , DOI: 10.1016/j.jinorgbio.2020.111275
Dorota Dudek 1 , Adriana Miller 1 , Sara Draghi 2 , Daniela Valensin 2 , Aleksandra Mikołajczyk 3 , Agnieszka Matera-Witkiewicz 3 , Danuta Witkowska 4 , Kamila Stokowa-Sołtys 1 , Magdalena Rowińska-Żyrek 1
Affiliation  

Often, in the search for a highly defined scientific phenomenon, a different one becomes apparent. This was also the case of this work, in the scope of which we planned to search for metal-enhanced, novel antibacterial/antifungal compounds. Instead, we denied the existence of such and revealed the details of the bioinorganic chemistry of Zn(II)-alloferon complexes. Zinc(II) complexes of alloferon 1 and 2, ligands with a sequential difference of one amino acid only, show a substantially different coordination pattern at physiological pH. In the case of Zn(II)-alloferon 1 species, a histamine-like binding mode is observed (N-terminal amine and imidazole of His1) and the coordination sphere is completed with the imidazole nitrogens of His6 and His9; His12 is not involved in binding. In the case of Zn(II)-alloferon 2, the N-terminal amine and all the three imidazoles present in the sequence participate in the coordination, however, with the chemical shift of His5 being less affected than those of other imidazoles. The histamine-like binding in Zn(II)-alloferon 1 complex strongly enhances its thermodynamic stability in comparison to the His-1 lacking alloferon 2 analogue. Despite previous reports on the antibacterial and antifungal activity of alloferon 1, no such activity was detected, neither for alloferon 1 and 2, nor for their Zn(II) complexes.



中文翻译:

锌(II)-阿洛法仑配合物–相似的序列,不同的配位模式,无抗菌活性

通常,在寻找一种高度定义的科学现象时,显然会出现另一种现象。这项工作也是如此,我们计划在此范围内寻找金属增强的新型抗菌/抗真菌化合物。取而代之的是,我们否认了此类化合物的存在,并揭示了Zn(II)-Alloferon配合物的生物无机化学细节。Alloferon 1和2的配体的锌(II)配合物仅具有一个氨基酸的顺序差异,在生理pH值下显示出显着不同的配位模式。在Zn(II)-Alloferon 1物种的情况下,观察到组胺样结合模式(His1的N端胺和咪唑),配位球由His6和His9的咪唑氮原子完成。His12不参与绑定。如果是Zn(II)-Alloferon 2,N-末端胺和序列中存在的所有三种咪唑都参与配位,但是,His5的化学位移受到的影响小于其他咪唑。与缺少Alloferon 2类似物的His-1相比,Zn(II)-alloferon 1复合物中的组胺样结合极大地增强了其热力学稳定性。尽管先前已有关于Alloferon 1的抗菌和抗真菌活性的报道,但未检测到Alloferon 1和2以及它们的Zn(II)复合物的这种活性。与缺少Alloferon 2类似物的His-1相比,Zn(II)-alloferon 1复合物中的组胺样结合极大地增强了其热力学稳定性。尽管先前已有关于Alloferon 1的抗菌和抗真菌活性的报道,但未检测到Alloferon 1和2以及它们的Zn(II)复合物的这种活性。与缺少Alloferon 2类似物的His-1相比,Zn(II)-alloferon 1复合物中的组胺样结合极大地增强了其热力学稳定性。尽管先前已有关于Alloferon 1的抗菌和抗真菌活性的报道,但未检测到Alloferon 1和2以及它们的Zn(II)复合物的这种活性。

更新日期:2020-10-13
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