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利用酪氨酸酶在酸性条件下合成可溶性黑色素纳米颗粒及其表征。

Synthesis of soluble melanin nanoparticles under acidic conditions using tyrosinase and their characterization.

作者信息

Kim Hyun, Lee Uk-Jae, Song Hanbit, Lee Jeongchan, Song Won-Suk, Noh Heewon, Kang Min-Ho, Kim Beom-Seok, Park Jungwon, Hwang Nathaniel S, Kim Byung-Gee

机构信息

School of Chemical and Biological Engineering, Seoul National University Seoul 08826 Republic of Korea

Institute of Molecular Biology and Genetics, Seoul National University Seoul 08826 Republic of Korea.

出版信息

RSC Adv. 2022 Jun 13;12(27):17434-17442. doi: 10.1039/d2ra01276f. eCollection 2022 Jun 7.

Abstract

Melanin nanoparticles (MNPs) used for biomedical applications are often synthesized the chemical auto-oxidation of catecholic monomers such as dopamine and 3,4-dihydroxyphenylalanine (DOPA) under alkaline conditions. However, the synthetic method for the chemical synthesis of MNP (cMNP) is relatively straightforward and more robust to control their homogenous particle size and morphology than the corresponding enzymatic synthetic methods. In this study, we demonstrated that the simple enzymatic synthesis of MNPs (eMNPs) with homogenous and soluble (<20 nm diameter) properties is possible using dopamine and tyrosinase (Ty) under acidic conditions (, pH 3.0). Ty was highly reactive under pH 5.0, where the natural and chemical oxidation of catechol is complex, and thus melanin was synthesized the hydroxylation of phenolic substrates. The detailed chemical analysis and characterization of the physical properties of the eMNPs confirmed the higher preservation of the catechol and primary amine moieties in the monomer substrate such as dopamine under acidic conditions. The eMNPs showed enhanced antioxidant activity and conferred stickiness to the formed hydrogel compared to the chemical auto-oxidation method owing to the large number of hydroxyl groups remaining such as catechol and quinone moieties. Because of these advantages and characteristics, the synthesis of MNPs using Ty under acidic conditions can open a new path for their biomedical applications.

摘要

用于生物医学应用的黑色素纳米颗粒(MNPs)通常是通过儿茶酚单体(如多巴胺和3,4-二羟基苯丙氨酸(DOPA))在碱性条件下的化学自氧化合成的。然而,与相应的酶促合成方法相比,化学合成MNP(cMNP)的合成方法相对简单,并且在控制其均匀粒径和形态方面更具稳健性。在本研究中,我们证明了在酸性条件下(pH 3.0)使用多巴胺和酪氨酸酶(Ty)可以简单地酶促合成具有均匀且可溶(直径<20 nm)特性的MNPs(eMNPs)。Ty在pH 5.0时具有高反应性(此时儿茶酚的自然氧化和化学氧化较为复杂),因此黑色素是通过酚类底物的羟基化合成的。对eMNPs物理性质的详细化学分析和表征证实,在酸性条件下,单体底物(如多巴胺)中的儿茶酚和伯胺部分得到了更高程度的保留。与化学自氧化方法相比,由于eMNPs中保留了大量如儿茶酚和醌部分的羟基,其抗氧化活性增强,并且赋予形成的水凝胶粘性。由于这些优点和特性,在酸性条件下使用Ty合成MNPs可为其生物医学应用开辟一条新途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e05d/9189705/4345b314f9c3/d2ra01276f-f1.jpg

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