Journal
CHEMISTRY OF MATERIALS
Volume 26, Issue 23, Pages 6743-6751Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm5030553
Keywords
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Funding
- ACS-PRF [52877DNI10]
- Colorado School of Mines
- Renewable Energy Materials Research Science and Engineering Center [DMR-0820518]
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1200547] Funding Source: National Science Foundation
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Colloidal iron pyrite nanocrystals (or FeS2 NC inks) are desirable as active materials in lithium ion batteries and photovoltaics and are particularly suitable for large-scale, roll-to-roll deposition or inkjet printing. However, to date, FeS2 NC inks have only been synthesized using the hot-injection technique, which requires air-free conditions and may not be desirable at an industrial scale. Here, we report the synthesis of monodisperse, colloidal, spherical, and phase-pure FeS2 NCs of 5.5 +/- 0.3 nm in diameter via a scalable solvothermal method using iron diethyldithiocarbamate as the precursor, combined with a postdigestive ripening process. The phase purity and crystallinity are determined using X-ray diffraction, transmission electron microscopy, far-infrared spectroscopy, and Raman spectroscopy techniques. Through this study, a hypothesis has been verified that solvothermal syntheses can also produce FeS2 NC inks by incorporating three experimental conditions: high solubility of the precursor, efficient mass transport, and sufficient stabilizing ligands. The addition of ligands and stirring decrease the NC size and led to a narrow size distribution. Moreover, using density functional theory calculations, we have identified an acid-mediated decomposition of the precursor as the initial and critical step in the synthesis of FeS2 from iron diethyldithiocarbamate.
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