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A Spectroscopic and Computational Structure-Function Study of Biosilicification Peptides

生物硅化肽的光谱和计算结构功能研究

基本信息

批准号：
1715123
负责人：
Gary Drobny
金额：
$ 67.89万
依托单位：
University of Washington
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-08-01 至 2021-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1715123&HistoricalAwards=false
关键词：
Spectroscopic Computational Structure Function Study

项目摘要

Metal oxides including silicon oxide (SiO2, silica) and titanium oxide (TiO2, titania) have numerous applications as insulators, textile coatings, catalysts, chemical decontaminants, solar cell components, medical/dental implants and chemical sensors. Industrial synthesis and morphological control of these important hard materials requires extremes in temperature, pressure and pH and are thus energetically demanding. In contrast, biological organisms accomplish impressive feats of mineral oxide production with precise control over morphology that is virtually unmatched by industrial approaches, and do so at ambient temperature, pressure and at physiological pH in a process called biomineralization. Biogenic silica (i.e. biosilica) is produced in gigaton quantities annually by the diatom, a marine microalgae characterized by an intricately decorated cell wall that is composed of organic material and silica. Diatoms take in silicon in dissolved form, and convert it to elaborate silica structures, in an as yet poorly understood process where proteins and other organic polymers are believed play important roles as catalysts and templates for silica formation. This research is aimed at understanding the specific roles played by proteins that are used by diatoms to form silica, with the immediate goal of making smaller, and less expensive molecules that imitate the diatom's ability to control silica formation under mild conditions. The long-term goal is to use similarly designed small molecules to effect the controlled formation of non-biological oxides like TiO2. This project will provide training for young scientists and engineers in the use of spectroscopic and computational techniques to elucidate structure-function relationships in biomaterials.The research will utilize solid state NMR (ssNMR), advanced non-equilibrium molecular dynamics (MD) computations, and novel chemical synthesis techniques, to determine the molecular structural properties and interactions that underlie the silicifying activities of naturally-occurring peptides. Initial study will be focused on modified and unmodified forms of the R5 peptide, derived from the bio-silicification protein silaffin of the diatom species Cylindrotheca fusiformis. Specific questions that this research project will address include: 1. Do unmodified silicifying peptide domain derived (e.g. R5) assume specific secondary structures that promote peptide-peptide interactions which in turn lead to formation of higher order structures? 2. What is the nature of peptide-silica interactions? 3. How do amino acid modifications influence peptide structure and peptide-peptide interactions in silica, and, most importantly, how do these modifications affect peptide-silica interactions? 4. Can R5, that induce silica formation, also induce formation of non-biological oxides like TiO2. Are the structural principles used by R5 to form silica similar to the principles it uses to form other oxides? Answers to these questions will provide structure-based principles for the design of peptides and other small molecules that can mimic in vitro the silicifying activities of naturally occurring proteins like silaffin.

金属氧化物包括二氧化硅(二氧化硅、二氧化硅)和二氧化钛(二氧化钛、二氧化钛)，在绝缘体、纺织涂料、催化剂、化学去污剂、太阳能电池组件、医疗/牙科植入物和化学传感器等方面有着广泛的应用。工业合成和形态控制这些重要的硬材料需要极端的温度、压力和pH，因此能量要求很高。相比之下，生物有机体实现了令人印象深刻的矿物氧化物生产壮举，其对形态的精确控制几乎是工业方法所无法比拟的，而且是在常温、常压和生理pH下通过一种称为生物矿化的过程做到这一点的。硅藻是一种海洋微藻，其特征是由有机材料和二氧化硅组成的复杂装饰的细胞壁，每年产生数十亿吨的生物硅(即生物硅)。硅藻以溶解的形式吸收硅，并将其转化为精细的二氧化硅结构，这一过程迄今知之甚少，蛋白质和其他有机聚合物被认为在二氧化硅形成的催化剂和模板中发挥了重要作用。这项研究旨在了解硅藻用来形成二氧化硅的蛋白质所起的特定作用，直接目标是制造更小、更便宜的分子，模仿硅藻在温和条件下控制二氧化硅形成的能力。长期目标是使用类似设计的小分子来控制像二氧化钛这样的非生物氧化物的形成。该项目将为年轻的科学家和工程师提供使用光谱和计算技术来阐明生物材料中结构-功能关系的培训。该研究将利用固体核磁共振(SsNMR)、先进的非平衡分子动力学(MD)计算和新的化学合成技术来确定天然多肽硅化活性的分子结构性质和相互作用。最初的研究将集中在R5肽的修饰和未修饰形式上，R5肽来自硅藻物种Cylindrotheca fusiformis的生物硅化蛋白silaffin。本研究项目将解决的具体问题包括：1.未修饰的硅化多肽结构域(例如R5)是否具有促进肽-肽相互作用进而导致更高级结构形成的特定二级结构？2.肽-硅相互作用的本质是什么？3.氨基酸修饰如何影响硅中的肽结构和肽-肽相互作用，最重要的是，这些修饰如何影响肽-硅相互作用？4.诱导硅形成的R5是否也能诱导像二氧化钛这样的非生物氧化物的形成。R5用来形成二氧化硅的结构原理与它用来形成其他氧化物的原理相似吗？对这些问题的回答将为多肽和其他小分子的设计提供基于结构的原理，这些小分子可以在体外模拟自然产生的蛋白质(如silaffin)的硅化活性。

项目成果

期刊论文数量（13）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Solid state deuterium NMR study of LKα14 peptide aggregation in biosilica

DOI：
10.1116/1.4986907
发表时间：
2017-06-01
期刊：
BIOINTERPHASES
影响因子：
2.1
作者：
Ferreira, Helen E.;Drobny, Gary P.
通讯作者：
Drobny, Gary P.

Backbone Structure of Diatom Silaffin Peptide R5 in Biosilica Determined by Combining Solid-State NMR with Theoretical Sum-Frequency Generation Spectra.

通过结合固态 NMR 与理论和频生成光谱测定生物二氧化硅中硅藻硅蜡肽 R5 的主链结构。

DOI：
发表时间：
2021
期刊：
Journal of Physical Chemistry Letters
影响因子：
5.7
作者：
Steven Joop Roeters;R. Mertig;Helmut Lutz;Adrienne M. Roehrich;G. Drobny;T. Weidner
通讯作者：
T. Weidner

Investigating the Role of Phosphorylation in the Binding of Silaffin Peptide R5 to Silica with Molecular Dynamics Simulations