Title: Thermodynamic Driving Force in the Spontaneous Formation of Inorganic Nanoparticle Solutions

Abstract

Nanoparticles are the bridge between the molecular and the macroscopic worlds. The growing number of commercial applications for nanoparticles spans from consumer products to new frontiers of medicine and next-generation optoelectronic technology. They are most commonly deployed in the form of a colloid, or “ink”, which are formulated with solvents, surfactants, and electrolytes to kinetically prevent the solid particulate phase from reaching the thermodynamically favored state of separate solid and liquid phases. In this work, we theoretically determine the thermodynamic requirements for forming a single-phase solution of spherical particles and engineer a model system to experimentally demonstrate the spontaneous formation of solutions composed of only solvent and bare inorganic nanoparticles. We show molecular interactions at the nanoparticle interface are the driving force in high-concentration nanoparticle solutions. The work establishes a regime where inorganic nanoparticles behave as molecular solutes as opposed to kinetically stable colloids, which has far-reaching implications for the future design and deployment of nanomaterial technologies.

Authors:

Wheeler, Lance M.  ^[1];

• Search DOE PAGES for author "Wheeler, Lance M."
• Search DOE PAGES for ORCID "0000-0002-1685-8242"

Kramer, Nicolaas J. ^[1]; Kortshagen, Uwe R.  ^[1]

• Search DOE PAGES for author "Kortshagen, Uwe R."
• Search DOE PAGES for ORCID "0000-0001-5944-3656"

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+ Show Author Affiliations

1. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Mechanical Engineering

Publication Date:

Mon Feb 26 00:00:00 EST 2018

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1470564

Grant/Contract Number:  

AC52-06NA25396

Resource Type:

Accepted Manuscript

Journal Name:

Nano Letters

Additional Journal Information:

Journal Volume: 18; Journal Issue: 3; Related Information: CASP partners with Los Alamos National Laboratory (lead); University of California, Irvine; University of Colorado; Colorado School of Mines; George Mason University; Los Alamos National Laboratory; University of Minnesota; National Renewable Energy Laboratory; Journal ID: ISSN 1530-6984

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 42 ENGINEERING; solar (photovoltaic); solar (fuels); solid state lighting; bio-inspired; electrodes - solar; defects; charge transport; materials and chemistry by design; optics; synthesis (novel materials); synthesis (scalable processing)