Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes

Nayak, Binay P.; Kim, Hyeong Jin; Travesset, Alex; Vaknin, David; Mallapragada, Surya K.; Wang, Wenjie

doi:10.1021/acs.jpcc.3c05722

Tuning Self-Assembly of Gold Nanoparticles Grafted with Charged Polymers by Varying Temperature and Electrolytes

Journal Article · Thu Dec 14 00:00:00 EST 2023 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.3c05722· OSTI ID:2248059

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Ames Lab., and Iowa State Univ., Ames, IA (United States)
Ames Laboratory (AMES), Ames, IA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: 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)

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358

OSTI ID:: 2248059

Report Number(s):: IS-J--11,220

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 51 Vol. 127; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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