Rational Design of Novel Biomimetic Sequence-Defined Polymers for Mineralization Applications

作者：Kaylyn Torkelson, Nada Y. Naser, Xin Qi, Zhiliang Li, Wenchao Yang, Karthik Pushpavanam, Chun‐Long Chen, François Baneyx, Jim Pfaendtner · 发表于：Chemistry of Materials · 年份：2024 · DOI：10.1021/acs.chemmater.3c02216 · 被引用次数：12 · 研究领域：Diatoms and Algae Research、Calcium Carbonate Crystallization and Inhibition、Marine Sponges and Natural Products

Silica biomineralization is a naturally occurring process, wherein organisms use proteins and other biological structures to direct the formation of complex, hierarchical nanostructures. Discovery and characterization of such proteins and their underlying mechanisms spurred significant efforts to identify routes for biomimetic mineralization that reproduce the exquisite shapes and size selectivities found in nature. A common strategy has been the use of short peptide sequences with chemistry mimicking those found in natural systems, such as the use of the silaffin-derived R5 peptide. While progress has been made using this approach, there are many limitations that have prevented breakthroughs in biomimicry. To advance our ability to use charged macromolecules for silica formation, we propose to use sequence-defined synthetic polymers known as peptoids, or N-substituted polyglycines, which present significant capability for the precise tuning of sequence and structure beyond what can often be achieved with peptides alone. This study presents a computationally predicted design of these polymers that leads to the controlled formation of silica nanomaterials. We investigate surface adsorption and the mineralization process through analysis of binding mechanisms and energetics of the R5 system. Next, we synthesized two R5-inspired peptoids and validated our prediction in the design of mineralization polymers through characterization using surface plasmon resonance and electron mic...