Aqueous Superparamagnetic Magnetite Dispersions with Ultrahigh Initial Magnetic Susceptibilities

Fei, Yunping; Iqbal, Muhammad; Kong, Seong D.; Xue, Zheng; McFadden, Charles P.; Guillet, Jesse L.; Doerrer, Linda H.; Alp, Esen E.; Bi, Wenli; Lu, Yi; Dandamudi, Chola B.; Ranganath, Prashant J.; Javier, Kevin J.; Ahmadian, Mohsen; Ellison, Christopher J.; Johnston, Keith P.

doi:10.1021/acs.langmuir.7b03702

Title: Aqueous Superparamagnetic Magnetite Dispersions with Ultrahigh Initial Magnetic Susceptibilities

Journal Article · 20 December 2017 · Langmuir

DOI: https://doi.org/10.1021/acs.langmuir.7b03702 · OSTI ID:1459893

Fei, Yunping ^[1]; Iqbal, Muhammad ^[1]; Kong, Seong D. ^[1]; Xue, Zheng ^[1]; McFadden, Charles P. ^[1]; Guillet, Jesse L. ^[2];

^[2]; Alp, Esen E. ^[3]; Bi, Wenli ^[3]; Lu, Yi ^[1]; Dandamudi, Chola B. ^[1]; Ranganath, Prashant J. ^[1]; Javier, Kevin J. ^[1]; Ahmadian, Mohsen ^[4];

^[1];

^[1]

Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
Boston Univ., MA (United States). Dept. of Chemistry
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Univ. of Texas, Austin, TX (United States). Advanced Energy Consortium & Bureau of Economic Geology

Superparamagnetic nanoparticles with a high initial magneti susceptibility χo are of great interest in a wide variety of chemical, biomedical, electronic, and subsurface energy applications. In order to achieve the theoretically predicted increase in χ_o with the cube of the magnetic diameter, new synthetic techniques are needed to control the crystal structure, particularly for magnetite nanoparticles larger than 10 nm. Aqueous magnetite dispersions (Fe₃O₄) with a χ_o of 3.3 (dimensionless SI units) at 1.9 vol %, over 3- to 5-fold greater than those reported previously, were produced in a one-pot synthesis at 210 °C and ambient pressure via thermal decomposition of Fe(II) acetate in triethylene glycol (TEG). The rapid nucleation and focused growth with an unusually high precursor-to-solvent molar ratio of 1:12 led to primary particles with a volume average diameter of 16 nm and low polydispersity according to TEM. The morphology was a mixture of stoichiometric and substoichiometric magnetite according to X-ray diffraction (XRD) and Mössbauer spectroscopy. Finally, the increase in χ_o with the cube of magnetic diameter as well as a saturation magnetization approaching the theoretical limit may be attributed to the highly crystalline structure and very small nonmagnetic layer (~1 nm) with disordered spin orientation on the surface.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Welch Foundation

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1459893

Journal Information:: Langmuir, Vol. 34, Issue 2; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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