2D/1D nanocomposites for energy storage applications
Synthesis and Properties of Functional Materials
Final Report Abstract
In summary, the study presents an additive-free exfoliation method for six different metal thiophosphates in an inert atmosphere, allowing investigation of their inherent nanomaterial properties while excluding oxidation effects. Utilizing cascade centrifugation, the nanomaterials were size-selected, yielding fractions with narrowed size and thickness distributions. TEM measurements on these size-selected nanomaterials revealed high crystallinity and expected elemental composition across fractions representative of large, intermediate, and small nanosheets. Statistical evaluation of nanosheet size and thickness distributions for each fraction show similar average dimensions, confirming the importance of anisotropic binding energy in nanosheet morphology and exfoliability, consistent with current understanding. Additionally, size-dependent optical properties were studied using absorbance and extinction spectroscopy for three representatives of the material class: NiPS3, FePS3 and MnPS3, which demonstrates similar changes across all materials. This allowed to establish empirical correlations between size/thickness information and peak intensity ratios/positions, respectively, deriving metrics for average nanosheet size and thickness. Moreover, the shift rate of excitonic transitions scales with bulk exciton resonance, consistent with previous findings on transition metal dichalcogenides, which is an intriguing result, but requires additional experiments before conclusions can be drawn. Our study also assessed the size-dependent environmental stability of the same three materials utilizing photo spectroscopic measurements. This allows to elucidate degradation mechanisms and to compare their stability to black phosphorus, where similar data was available from previous studies. The results suggest limited practicality for metal thiophosphates, particularly for catalytic applications. Furthermore, we identified magnetic correlations in antiferromagnetic nanomaterials through cryo-Raman and magnetic susceptibility measurements in a wet chemical environment. Demonstrating the materials' application in sodium ion batteries, we achieved near-theoretical capacities, highlighting the high crystal quality of the nanomaterials, in line with Raman and TEM measurements. Overall, the work conducted on metal thiophosphates provides a foundational understanding for researchers interested in exploiting the optical, electrochemical, and magnetic properties of metal thiophosphate nanosheets. It offers guidance for fabricating air-sensitive nanosheets with intrinsic material properties and assessing their stability across different environments. Additionally, our experiments provide universally applicable insights into size-dependent properties and environmental stability, facilitating comparisons across diverse material systems and chemical environments.
Publications
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Exfoliablity, magnetism, energy storage and stability of metal thiophosphate nanosheets made in liquid medium. 2D Materials, 10(2), 024003.
Synnatschke, Kevin; van Dinter, Jonas; Müller, Alina; Tiede, David; Spillecke, Lena; Shao, Shouqi; Kelly, Daniel; Konecny, Jan; Konkena, Bharathi; McCrystall, Mark; Saigal, Nihit; Wurstbauer, Ursula; Bensch, Wolfgang; Sofer, Zdeněk; Coleman, Jonathan N.; Klingeler, Rüdiger; Haigh, Sarah J. & Backes, Claudia
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Solution-Processed NiPS3 Thin Films from Liquid Exfoliated Inks with Long-Lived Spin-Entangled Excitons. ACS Nano, 17(11), 10423-10430.
Shcherbakov, Andrii; Synnatschke, Kevin; Bodnar, Stanislav; Zerhoch, Jonathan; Eyre, Lissa; Rauh, Felix; Heindl, Markus W.; Liu, Shangpu; Konecny, Jan; Sharp, Ian D.; Sofer, Zdeněk; Backes, Claudia & Deschler, Felix
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Sonication-assisted liquid exfoliation and size-dependent properties of magnetic two-dimensional α-RuCl3. Journal of Physics D: Applied Physics, 56(27), 274001.
Synnatschke, Kevin; Jonak, Martin; Storm, Alexander; Laha, Sourav; Köster, Janis; Petry, Julian; Ott, Steffen; Szydłowska, Beata; Duesberg, Georg S.; Kaiser, Ute; Klingeler, Rüdiger; Lotsch, Bettina V. & Backes, Claudia
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Sonication-assisted liquid phase exfoliation of two-dimensional CrTe3 under inert conditions. Ultrasonics Sonochemistry, 98, 106528.
Synnatschke, Kevin; Moses, Badlyan Narine; Wrzesińska, Angelika; Lozano, Onrubia Guillermo; Hansen, Anna–Lena; Wolff, Stefan; Tornatzky, Hans; Bensch, Wolfgang; Vaynzof, Yana; Maultzsch, Janina & Backes, Claudia
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Long lived photogenerated charge carriers in few-layer transition metal dichalcogenides obtained from liquid phase exfoliation. Nanoscale Advances, 6(4), 1074-1083.
Morabito, Floriana; Synnatschke, Kevin; Mehew, Jake Dudley; Varghese, Sebin; Sayers, Charles James; Folpini, Giulia; Petrozza, Annamaria; Cerullo, Giulio; Tielrooij, Klaas-Jan; Coleman, Jonathan; Nicolosi, Valeria & Gadermaier, Christoph
