Interfacial Self-Assembly of Polyelectrolyte-Capped Gold Nanoparticles

Zhang, Honghu; Nayak, Srikanth; Wang, Wenjie; Mallapragada, Surya; Vaknin, David

doi:10.1021/acs.langmuir.7b02359

Interfacial Self-Assembly of Polyelectrolyte-Capped Gold Nanoparticles

Journal Article · Fri Oct 06 00:00:00 EDT 2017 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.7b02359· OSTI ID:1409368

Zhang, Honghu ^[1]; Nayak, Srikanth ^[1]; Wang, Wenjie ^[2]; Mallapragada, Surya ^[1]; ^[1]

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

Here, we report on pH- and salt-responsive assembly of nanoparticles capped with polyelectrolytes at vapor–liquid interfaces. Two types of alkylthiol-terminated poly(acrylic acid) (PAAs, varying in length) are synthesized and used to functionalize gold nanoparticles (AuNPs) to mimic similar assembly effects of single-stranded DNA-capped AuNPs using synthetic polyelectrolytes. Using surface-sensitive X-ray scattering techniques, including grazing incidence small-angle X-ray scattering (GISAXS) and X-ray reflectivity (XRR), we demonstrate that PAA-AuNPs spontaneously migrate to the vapor–liquid interfaces and form Gibbs monolayers by decreasing the pH of the suspension. The Gibbs monoalyers show chainlike structures of monoparticle thickness. The pH-induced self-assembly is attributed to the protonation of carboxyl groups and to hydrogen bonding between the neighboring PAA-AuNPs. In addition, we show that adding MgCl₂ to PAA-AuNP suspensions also induces adsorption at the interface and that the high affinity between magnesium ions and carboxyl groups leads to two- and three-dimensional clusters that yield partial surface coverage and poorer ordering of NPs at the interface. We also examine the assembly of PAA-AuNPs in the presence of a positively charged Langmuir monolayer that promotes the attraction of the negatively charged capped NPs by electrostatic forces. Our results show that synthetic polyelectrolyte-functionalized nanoparticles exhibit interfacial self-assembly behavior similar to that of DNA-functionalized nanoparticles, providing a pathway for nanoparticle assembly in general.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1409368

Alternate ID(s):: OSTI ID: 1438851

Report Number(s):: IS-J--9499

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 43 Vol. 33; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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