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Fe(III) 和 Cu(II) 微过氧化物酶-11 与脂质正电荷界面相互作用的结构和催化作用。

Structure and Catalysis of Fe(III) and Cu(II) Microperoxidase-11 Interacting with the Positively Charged Interfaces of Lipids.

机构信息

Universidade Federal do ABC, Santo André 09210-170, SP, Brazil.

Universidade de São Paulo, Instituto de Física de São Carlos, São Carlos 13400-970, SP, Brazil.

出版信息

Molecules. 2017 Jul 26;22(8):1212. doi: 10.3390/molecules22081212.

DOI:10.3390/molecules22081212
PMID:28933729
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6151982/
Abstract

Numerous applications have been described for microperoxidases (MPs) such as in photoreceptors, sensing, drugs, and hydrogen evolution. The last application was obtained by replacing Fe(III), the native central metal, by cobalt ion and inspired part of the present study. Here, the Fe(III) of MP-11 was replaced by Cu(II) that is also a stable redox state in aerated medium, and the structure and activity of both MPs were modulated by the interaction with the positively charged interfaces of lipids. Comparative spectroscopic characterization of Fe(III) and Cu(II)MP-11 in the studied media demonstrated the presence of high and low spin species with axial distortion. The association of the Fe(III)MP-11 with CTAB and Cu(II)MP-11 with DODAB affected the colloidal stability of the surfactants that was recovered by heating. This result is consistent with hydrophobic interactions of MPs with DODAB vesicles and CTAB micelles. The hydrophobic interactions decreased the heme accessibility to substrates and the Fe(III) MP-11catalytic efficiency. Cu(II)MP-11 challenged by peroxides exhibited a cyclic Cu(II)/Cu(I) interconversion mechanism that is suggestive of a mimetic Cu/ZnSOD (superoxide dismutase) activity against peroxides. Hydrogen peroxide-activated Cu(II)MP-11 converted Amplex Red to dihydroresofurin. This study opens more possibilities for technological applications of MPs.

摘要

已经有许多应用描述了微过氧化物酶（MPs），如在光感受器、传感、药物和氢的演化中。最后一个应用是通过用钴离子取代天然中心金属铁（III）得到的，这激发了本研究的一部分。在这里，MP-11 的 Fe(III) 被 Cu(II)取代，Cu(II)在有氧介质中也是一种稳定的氧化还原态，并且两种 MPs 的结构和活性都通过与带正电荷的脂质界面的相互作用来调节。在研究的介质中对 Fe(III)和 Cu(II)MP-11 的比较光谱特性表明存在具有轴向扭曲的高自旋和低自旋物种。Fe(III)MP-11 与 CTAB 和 Cu(II)MP-11 与 DODAB 的结合影响了表面活性剂的胶体稳定性，通过加热可以恢复这种稳定性。这一结果与 MPs 与 DODAB 囊泡和 CTAB 胶束的疏水相互作用一致。疏水相互作用降低了血红素对底物的可及性和 Fe(III)MP-11 的催化效率。过氧化物挑战的 Cu(II)MP-11 表现出循环 Cu(II)/Cu(I)相互转化机制，这表明它对过氧化物具有类似 Cu/ZnSOD（超氧化物歧化酶）的活性。过氧化氢激活的 Cu(II)MP-11 将 Amplex Red 转化为二氢 Resofurin。这项研究为 MPs 的技术应用开辟了更多的可能性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/8e614eb4c095/molecules-22-01212-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/3c057399693e/molecules-22-01212-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/a21e610d29a3/molecules-22-01212-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/cb33a809d860/molecules-22-01212-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/e5df55757013/molecules-22-01212-g004a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/1043535d07b4/molecules-22-01212-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/e117769f9da4/molecules-22-01212-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/1a2ff6ba7d36/molecules-22-01212-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/92591172073e/molecules-22-01212-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/468e197eefc8/molecules-22-01212-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/8e614eb4c095/molecules-22-01212-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/3c057399693e/molecules-22-01212-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/a21e610d29a3/molecules-22-01212-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/cb33a809d860/molecules-22-01212-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/e5df55757013/molecules-22-01212-g004a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/1043535d07b4/molecules-22-01212-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/e117769f9da4/molecules-22-01212-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/1a2ff6ba7d36/molecules-22-01212-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/92591172073e/molecules-22-01212-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/468e197eefc8/molecules-22-01212-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/689c/6151982/8e614eb4c095/molecules-22-01212-g010.jpg

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