使用具有设计后翻译修饰的硅藻肽生产的二氧化硅纳米结构,Advanced Functional Materials

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使用具有设计后翻译修饰的硅藻肽生产的二氧化硅纳米结构
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2020-06-03 , DOI: 10.1002/adfm.202000849
Andrea K. Wallace ₁ , Nicolas Chanut ₂ , Christopher A. Voigt ₁

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硅藻在环境条件下会产生复杂的图案化二氧化硅结构，该过程是由翻译后修饰的可形成硅酸的硅蜡肽启动的。设计这些肽将能够生产具有所需特性的二氧化硅纳米结构。但是，修改的功能效果了解得很少。在这里，大肠杆菌用于表达和修饰来自硅藻圆柱藻的重组silaffin R5肽。测试了38个酶的文库的R5修饰体外，从硅藻，人，酵母和细菌中鉴定出了活性甲基转移酶，激酶，乙酰基转移酶，氧化酶和肉豆蔻酰基转移酶。修饰的R5肽用于二氧化硅沉淀，并量化了其对粒径，形状，孔隙率和表面积的影响。设计体内途径共表达R5和修饰酶，所得肽用于成核尺寸（100-3500 nm），孔隙度（20-635 m ² g ^-1）受控的二氧化硅纳米结构），或嵌入黑色素。发现磷酸化减少了二氧化硅合成过程中对无机磷酸盐的需要。R5的同时甲基化和磷酸化导致较小的颗粒，需要较少的无机磷酸盐。受硅藻启发，翻译后修饰的肽的使用将能够控制环境条件下的二氧化硅形态，并可能在电子和光子学中得到应用。

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Silica Nanostructures Produced Using Diatom Peptides with Designed Post‐Translational Modifications

Diatoms produce intricately patterned silica structures under ambient conditions, a process initiated by post‐translationally modified silaffin peptides that nucleate silicic acid. Designing these peptides would enable the production of silica nanostructures with desired properties; however, the functional effects of modifications are poorly understood. Here, Escherichia coli is used to express and modify recombinant silaffin R5 peptide from the diatom Cylindrotheca fusiformis . A library of 38 enzymes is tested for R5 modifications in vitro, from which active methyltransferases, kinases, acetyltransferases, oxidases, and myristoyltransferases are identified from diatoms, humans, yeast, and bacteria. Modified R5 peptides are used for silica precipitation and the impacts on particle size, shape, porosity, and surface area are quantified. In vivo pathways are designed to coexpress R5 and a modifying enzyme and the resulting peptide is used to nucleate silica nanostructures with controlled size (100–3500 nm), porosity (20–635 m² g⁻¹), or embedded with melanin. It is found that phosphorylation reduces the need for inorganic phosphate during silica synthesis. The simultaneous methylation and phosphorylation of R5 leads to smaller particles requiring less inorganic phosphate. Inspired by diatoms, the use of post‐translationally modified peptides will enable the control of silica morphology under ambient conditions, with potential applications in electronics and photonics.

更新日期：2020-07-23

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