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Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes
Abstract
Here, we report on the assembly of gold nanoparticles (AuNPs, 5 and 10 nm core diameters) grafted with poly(ethylene glycol) (PEG) terminated with either positively (–NH2) or negatively charged (–COOH) end groups. We employ synchrotron-based small-angle X-ray scattering (SAXS) techniques to investigate the effect of electrolytes and temperature on the assembly and crystallization behavior of these grafted AuNPs. Our studies reveal that –NH2-grafted AuNPs spontaneously assemble into a layered hexagonal structure that deteriorates upon adding K2CO3 to the suspension. The hexagonal structure recovers after heating the same suspension above 60 °C. On the other hand, the COOH-terminated AuNPs remain dispersed in the suspensions and assemble and crystallize into a face-centered cubic structure only in the presence of K2CO3 at temperatures above 60 °C. Varying the pH of the –NH2-terminated AuNP suspensions induces short-range order (SRO) structures with a single characteristic length scale that shrinks upon heating. Similarly, SRO for the –COOH-terminated AuNP is realized only by lowering the pH. This study demonstrates the use of electrolytes and temperature on the surface charge of grafted AuNPs as knobs to tune self-assembly and crystallization.
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[2]
- Ames Lab., and Iowa State Univ., Ames, IA (United States)
- Ames Laboratory (AMES), Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
- OSTI Identifier:
- 2248059
- Report Number(s):
- IS-J-11,220
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- AC02-07CH11358; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 127; Journal Issue: 51; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemical structure; Diffraction; Electrolytes; Metal nanoparticles; Suspensions
Citation Formats
Nayak, Binay P., Kim, Hyeong Jin, Travesset, Alex, Vaknin, David, Mallapragada, Surya K., and Wang, Wenjie. Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes. United States: N. p., 2023.
Web. doi:10.1021/acs.jpcc.3c05722.
Nayak, Binay P., Kim, Hyeong Jin, Travesset, Alex, Vaknin, David, Mallapragada, Surya K., & Wang, Wenjie. Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes. United States. https://doi.org/10.1021/acs.jpcc.3c05722
Nayak, Binay P., Kim, Hyeong Jin, Travesset, Alex, Vaknin, David, Mallapragada, Surya K., and Wang, Wenjie. Thu .
"Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes". United States. https://doi.org/10.1021/acs.jpcc.3c05722.
@article{osti_2248059,
title = {Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes},
author = {Nayak, Binay P. and Kim, Hyeong Jin and Travesset, Alex and Vaknin, David and Mallapragada, Surya K. and Wang, Wenjie},
abstractNote = {Here, we report on the assembly of gold nanoparticles (AuNPs, 5 and 10 nm core diameters) grafted with poly(ethylene glycol) (PEG) terminated with either positively (–NH2) or negatively charged (–COOH) end groups. We employ synchrotron-based small-angle X-ray scattering (SAXS) techniques to investigate the effect of electrolytes and temperature on the assembly and crystallization behavior of these grafted AuNPs. Our studies reveal that –NH2-grafted AuNPs spontaneously assemble into a layered hexagonal structure that deteriorates upon adding K2CO3 to the suspension. The hexagonal structure recovers after heating the same suspension above 60 °C. On the other hand, the COOH-terminated AuNPs remain dispersed in the suspensions and assemble and crystallize into a face-centered cubic structure only in the presence of K2CO3 at temperatures above 60 °C. Varying the pH of the –NH2-terminated AuNP suspensions induces short-range order (SRO) structures with a single characteristic length scale that shrinks upon heating. Similarly, SRO for the –COOH-terminated AuNP is realized only by lowering the pH. This study demonstrates the use of electrolytes and temperature on the surface charge of grafted AuNPs as knobs to tune self-assembly and crystallization.},
doi = {10.1021/acs.jpcc.3c05722},
journal = {Journal of Physical Chemistry. C},
number = 51,
volume = 127,
place = {United States},
year = {Thu Dec 14 00:00:00 EST 2023},
month = {Thu Dec 14 00:00:00 EST 2023}
}
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