Understanding the formation mechanism of magnetic mesocrystals with (cryo-)electron microscopy

Giulia Mirabello, Arthur Keizer, Paul H.H. Bomans, András Kovács, Rafal E. Dunin-Borkowski, Nico A.J.M. Sommerdijk (Corresponding author), Heiner Friedrich (Corresponding author)

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Magnetite (Fe3O4) nanoaggregates with a flower-like morphology are considered promising materials in the field of magnetically induced hyperthermia in cancer therapy due to their good heating efficiency at low applied alternating magnetic fields. Although the structure and the magnetic state of such flower-like aggregates have been investigated previously, the mechanism that leads to the hierarchical morphology is still poorly understood. Here, we study the formation mechanism of Fe3O4 aggregates synthesized through the partial oxidation of ferrous hydroxide in the presence of poly(acrylic acid) by using cryogenic electron microscopy. The aggregates are formed through a multistep process involving first the conversion of ferrous hydroxide precursors in ∼5 nm primary particles that aggregate into ∼10 nm primary Fe3O4 crystals that finally arrange into the secondary mesocrystal structure. High-resolution electron tomography is used to show that the Fe3O4 mesocrystals are composed of ∼10 nm subunits, often showing a uniform crystallographic orientation resulting in single-crystal-like diffraction patterns. Furthermore, electron holography reveals that mesocrystals have a single magnetic domain despite polymeric interfaces between subunits being present throughout the mesocrystal. Our findings could be used to design materials with specific properties by modulating the morphology and/or magnetic state that is suitable for biomedical application.

Originele taal-2Engels
Pagina's (van-tot)7320-7328
Aantal pagina's9
TijdschriftChemistry of Materials
Volume31
Nummer van het tijdschrift18
DOI's
StatusGepubliceerd - 24 sep 2019

Vingerafdruk

Electron microscopy
carbopol 940
Electron holography
Ferrosoferric Oxide
Magnetic domains
Magnetite
Crystal orientation
Cryogenics
Diffraction patterns
Acrylics
Tomography
Single crystals
Magnetic fields
Heating
Oxidation
Crystals
Acids
Electrons
hydroxide ion

Citeer dit

Mirabello, Giulia ; Keizer, Arthur ; Bomans, Paul H.H. ; Kovács, András ; Dunin-Borkowski, Rafal E. ; Sommerdijk, Nico A.J.M. ; Friedrich, Heiner. / Understanding the formation mechanism of magnetic mesocrystals with (cryo-)electron microscopy. In: Chemistry of Materials. 2019 ; Vol. 31, Nr. 18. blz. 7320-7328.
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abstract = "Magnetite (Fe3O4) nanoaggregates with a flower-like morphology are considered promising materials in the field of magnetically induced hyperthermia in cancer therapy due to their good heating efficiency at low applied alternating magnetic fields. Although the structure and the magnetic state of such flower-like aggregates have been investigated previously, the mechanism that leads to the hierarchical morphology is still poorly understood. Here, we study the formation mechanism of Fe3O4 aggregates synthesized through the partial oxidation of ferrous hydroxide in the presence of poly(acrylic acid) by using cryogenic electron microscopy. The aggregates are formed through a multistep process involving first the conversion of ferrous hydroxide precursors in ∼5 nm primary particles that aggregate into ∼10 nm primary Fe3O4 crystals that finally arrange into the secondary mesocrystal structure. High-resolution electron tomography is used to show that the Fe3O4 mesocrystals are composed of ∼10 nm subunits, often showing a uniform crystallographic orientation resulting in single-crystal-like diffraction patterns. Furthermore, electron holography reveals that mesocrystals have a single magnetic domain despite polymeric interfaces between subunits being present throughout the mesocrystal. Our findings could be used to design materials with specific properties by modulating the morphology and/or magnetic state that is suitable for biomedical application.",
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Understanding the formation mechanism of magnetic mesocrystals with (cryo-)electron microscopy. / Mirabello, Giulia; Keizer, Arthur; Bomans, Paul H.H.; Kovács, András; Dunin-Borkowski, Rafal E.; Sommerdijk, Nico A.J.M. (Corresponding author); Friedrich, Heiner (Corresponding author).

In: Chemistry of Materials, Vol. 31, Nr. 18, 24.09.2019, blz. 7320-7328.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

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