Rational Design of Novel Biomimetic Sequence-Defined Polymers for Mineralization Applications
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- University of Washington, Seattle, WA (United States)
- University of Washington, Seattle, WA (United States); Dartmouth College, Hanover, NH (United States)
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Shandong University (China)
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Tianjin University (China)
- University of Washington, Seattle, WA (United States); Indian Institute of Technology Gandhinagar, Gujarat (India)
- University of Washington, Seattle, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- University of Washington, Seattle, WA (United States); North Carolina State University, Raleigh, NC (United States)
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 microscopy. Here, this computationally guided study holds great promise for designing new sequences with unprecedented control of the placement of chemical functional groups, thus allowing for further unraveling of silicification mechanisms and the eventual design of sequence-defined synthetic polymers leading to the predictive synthesis of nanostructured functional materials.
- Research Organization:
- Univ. of Washington, Seattle, WA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- Grant/Contract Number:
- SC0019288; AC05-76RL01830; NNCI-1542101
- OSTI ID:
- 2290446
- Journal Information:
- Chemistry of Materials, Vol. 36, Issue 2; ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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