Final Report for Fractionation and Separation of Polydisperse Nanoparticles into Distinct Monodisperse Fractions Using CO2 Expanded Liquids

Roberts, Chistopher

Auburn University

关键词: 77 Nanoscience And Nanotechnology;    Nanostructures;    99 General And Miscellaneous//Mathematics, Computing, And Information Science;    Particle Size Classifiers;    Organic Solvents;   

DOI  :  10.2172/935215
RP-ID  :  None
RP-ID  :  FG26-06NT42685
RP-ID  :  935215

美国|英语

来源: UNT Digital Library

【 摘 要 】

The overall objective of this project was to facilitate efficient fractionation and separation of polydisperse metal nanoparticle populations into distinct monodisperse fractions using the tunable solvent properties of gas expanded liquids. Specifically, the dispersibility of ligand-stabilized nanoparticles in an organic solution was controlled by altering the ligand-solvent interaction (solvation) by the addition of carbon dioxide (CO{sub 2}) gas as an antisolvent (thereby tailoring the bulk solvent strength) in a custom high pressure apparatus developed in our lab. This was accomplished by adjusting the CO{sub 2} pressure over the liquid dispersion, resulting in a simple means of tuning the nanoparticle precipitation by size. Overall, this work utilized the highly tunable solvent properties of organic/CO{sub 2} solvent mixtures to selectively size-separate dispersions of polydisperse nanoparticles (ranging from 1 to 20 nm in size) into monodisperse fractions ({+-}1nm). Specifically, three primary tasks were performed to meet the overall objective. Task 1 involved the investigation of the effects of various operating parameters (such as temperature, pressure, ligand length and ligand type) on the efficiency of separation and fractionation of Ag nanoparticles. In addition, a thermodynamic interaction energy model was developed to predict the dispersibility of different sized nanoparticles in the gas expanded liquids at various conditions. Task 2 involved the extension of the experimental procedures identified in task 1 to the separation of other metal particles used in catalysis such as Au as well as other materials such as semiconductor particles (e.g. CdSe). Task 3 involved using the optimal conditions identified in tasks 1 and 2 to scale up the process to handle sample sizes of greater than 1 g. An experimental system was designed to allow nanoparticles of increasingly smaller sizes to be precipitated sequentially in a vertical series of high pressure vessels by moving the liquid nanoparticle dispersion from the top vessel to the bottom vessel with corresponding CO{sub 2} pressure increases at each stage. For example, three fractions with average diameters of 7.00 nm, 4.35 nm, and 3.95 nm were recovered from a 20ml sample of Ag nanoparticles dispersed in hexane at pressures of 625 psi, 650 psi, >650 psi, respectively.