Time-Resolved SAXS Study of Polarity- and Surfactant-Controlled Superlattice Transformations of Oleate-Capped Nanocubes During Solvent Removal

Structural transformations and lattice expansion of oleate-capped iron oxide nanocube superlattices are studied by time-resolved small-angle X-ray scattering (SAXS) during solvent removal. The combination of conductor-like screening model for real solvents (COSMO-RS) theory with computational fluid dynamics (CFD) modeling provides information on the solvent composition and polarity during droplet evaporation. Evaporation-driven poor-solvent enrichment in the presence of free oleic acid results in the formation of superlattices with a tilted face-centered cubic (fcc) structure when the polarity reaches its maximum. The tilted fcc lattice expands subsequently during the removal of the poor solvent and eventually transforms to a regular simple cubic (sc) lattice during the final evaporation stage when only free oleic acid remains. Comparative studies show that both the increase in polarity as the poor solvent is enriched and the presence of a sufficient amount of added oleic acid is required to promote the formation of structurally diverse superlattices with large domain sizes.

Description

Funding Information: The authors acknowledge the Swedish Research Council (VR, grant numbers 2018–06378 and 2019–05624) for funding this work. This work was also supported by the Postdoctoral Researcher funding of Academy of Finland (330214), the New National Excellence Program Hungarian Ministry of Human Capacities (UNKP‐21‐5), and the Janos Bolyai Research Scholarship of the Hungarian Academy of Sciences. The authors thank Y. Zhong for assistance with TEM measurements, and M. Segad, and P. Munier, for assistance with the acquisition of SAXS data. The authors are also grateful to T. Plivelic from the CoSAXS beamline at MAX IV for providing the ultrasonic levitator and S. Disch from University of Cologne for providing the superball plugin mode in SasView. The authors acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III and The authors would like to thank W. Ohm for assistance using beamline P03. Beamtime was allocated for proposal I‐20180345 EC. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. This work benefited from the use of the SasView application, originally developed under NSF award DMR‐0520547. SasView also contains code developed with funding from the European Union's Horizon 2020 research and innovation program under the SINE2020 project, grant agreement No 654000. Z. P. Lv also offers sincere condolence to Dr. Long Cui, his former colleague and close friend, who passed away in a deplorable accident. Publisher Copyright: © 2022 The Authors. Small published by Wiley-VCH GmbH.

Keywords

anisotropic nanoparticles, small angle X-ray scattering, superlattice transformation, time-dependent measurements

DOI

10.1002/smll.202106768

Citation

Lv, Z P, Kapuscinski, M, Járvás, G, Yu, S & Bergström, L 2022, ' Time-Resolved SAXS Study of Polarity- and Surfactant-Controlled Superlattice Transformations of Oleate-Capped Nanocubes During Solvent Removal ', Small, vol. 18, no. 22, 2106768 . https://doi.org/10.1002/smll.202106768

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https://urn.fi/URN:NBN:fi:aalto-202208104529

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[article-cris] Perustieteiden korkeakoulu / SCI

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Time-Resolved SAXS Study of Polarity- and Surfactant-Controlled Superlattice Transformations of Oleate-Capped Nanocubes During Solvent Removal

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