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Title: Compact Peptoid Molecular Brushes for Nanoparticle Stabilization

Abstract

Controlling the interfaces and interactions of colloidal nanoparticles (NPs) via tethered molecular moieties is crucial for NP applications in engineered nanomaterials, optics, catalysis, and nanomedicine. Despite a broad range of molecular types explored, there is a need for a flexible approach to rationally vary the chemistry and structure of these interfacial molecules for controlling NP stability in diverse environments, while maintaining a small size of the NP molecular shell. Here, we demonstrate that low-molecular-weight, bifunctional comb-shaped, and sequence-defined peptoids can effectively stabilize gold NPs (AuNPs). The generality of this robust functionalization strategy was also demonstrated by coating of silver, platinum, and iron oxide NPs with designed peptoids. Each peptoid (PE) is designed with varied arrangements of a multivalent AuNP-binding domain and a solvation domain consisting of oligo-ethylene glycol (EG) branches. Among designs, a peptoid (PE5) with a diblock structure is demonstrated to provide a superior nanocolloidal stability in diverse aqueous solutions while forming a compact shell (similar to 1.5 nm) on the AuNP surface. We demonstrate by experiments and molecular dynamics simulations that PE5-coated AuNPs (PE5/AuNPs) are stable in select organic solvents owing to the strong PE5 (amine)-Au binding and solubility of the oligo-EG motifs. At the vapor-aqueous interface, wemore » show that PE5/AuNPs remain stable and can self-assemble into ordered 2D lattices. The NP films exhibit strong near-field plasmonic coupling when transferred to solid substrates.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [1];  [3]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  4. RMIT Univ., Melbourne, VIC (Australia)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1890433
Report Number(s):
BNL-223526-2022-JAAM
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
SC0012704; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 144; Journal Issue: 18; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; peptoid; interface; NP stability; phase transfer; self-assembly

Citation Formats

Wang, Shih-Ting, Zhang, Honghu, Xuan, Sunting, Nykypanchuk, Dmytro, Zhang, Yugang, Freychet, Guillaume, Ocko, Benjamin M., Zuckermann, Ronald N., Todorova, Nevena, and Gang, Oleg. Compact Peptoid Molecular Brushes for Nanoparticle Stabilization. United States: N. p., 2022. Web. doi:10.1021/jacs.2c00743.
Wang, Shih-Ting, Zhang, Honghu, Xuan, Sunting, Nykypanchuk, Dmytro, Zhang, Yugang, Freychet, Guillaume, Ocko, Benjamin M., Zuckermann, Ronald N., Todorova, Nevena, & Gang, Oleg. Compact Peptoid Molecular Brushes for Nanoparticle Stabilization. United States. https://doi.org/10.1021/jacs.2c00743
Wang, Shih-Ting, Zhang, Honghu, Xuan, Sunting, Nykypanchuk, Dmytro, Zhang, Yugang, Freychet, Guillaume, Ocko, Benjamin M., Zuckermann, Ronald N., Todorova, Nevena, and Gang, Oleg. Fri . "Compact Peptoid Molecular Brushes for Nanoparticle Stabilization". United States. https://doi.org/10.1021/jacs.2c00743. https://www.osti.gov/servlets/purl/1890433.
@article{osti_1890433,
title = {Compact Peptoid Molecular Brushes for Nanoparticle Stabilization},
author = {Wang, Shih-Ting and Zhang, Honghu and Xuan, Sunting and Nykypanchuk, Dmytro and Zhang, Yugang and Freychet, Guillaume and Ocko, Benjamin M. and Zuckermann, Ronald N. and Todorova, Nevena and Gang, Oleg},
abstractNote = {Controlling the interfaces and interactions of colloidal nanoparticles (NPs) via tethered molecular moieties is crucial for NP applications in engineered nanomaterials, optics, catalysis, and nanomedicine. Despite a broad range of molecular types explored, there is a need for a flexible approach to rationally vary the chemistry and structure of these interfacial molecules for controlling NP stability in diverse environments, while maintaining a small size of the NP molecular shell. Here, we demonstrate that low-molecular-weight, bifunctional comb-shaped, and sequence-defined peptoids can effectively stabilize gold NPs (AuNPs). The generality of this robust functionalization strategy was also demonstrated by coating of silver, platinum, and iron oxide NPs with designed peptoids. Each peptoid (PE) is designed with varied arrangements of a multivalent AuNP-binding domain and a solvation domain consisting of oligo-ethylene glycol (EG) branches. Among designs, a peptoid (PE5) with a diblock structure is demonstrated to provide a superior nanocolloidal stability in diverse aqueous solutions while forming a compact shell (similar to 1.5 nm) on the AuNP surface. We demonstrate by experiments and molecular dynamics simulations that PE5-coated AuNPs (PE5/AuNPs) are stable in select organic solvents owing to the strong PE5 (amine)-Au binding and solubility of the oligo-EG motifs. At the vapor-aqueous interface, we show that PE5/AuNPs remain stable and can self-assemble into ordered 2D lattices. The NP films exhibit strong near-field plasmonic coupling when transferred to solid substrates.},
doi = {10.1021/jacs.2c00743},
journal = {Journal of the American Chemical Society},
number = 18,
volume = 144,
place = {United States},
year = {Fri Apr 22 00:00:00 EDT 2022},
month = {Fri Apr 22 00:00:00 EDT 2022}
}

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