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Meyerson, Melissa L.

Publications and source records attributed to Meyerson, Melissa L..

5 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

High-Entropy Metal-Organic Frameworks (HEMOFs): A New Frontier in Materials Design for CO 2 Utilization

High-entropy materials (HEMs) emerged as promising candidates for a diverse array of chemical transformations, including CO 2 utilization. However, traditional HEMs catalysts are nonporous, limiting their activity to surface sites. Designing HEMs with intrinsic porosity can open the door toward enhanced reactivity while maintaining the many benefits of high configurational entropy. Here, in this study, a synergistic experimental, analytical, and theoretical approach to design the first high-entropy metal-organic frameworks (HEMOFs) derived from polynuclear metal clusters is implemented, a novel class of porous HEMs that is highly active for CO 2 fixation under mild conditions and short reaction times, outperforming existing heterogeneous catalysts. HEMOFs with up to 15 distinct metals are synthesized (the highest number of metals ever incorporated into a single MOF) and, for the first time, homogenous metal mixing within individual clusters is directly observed via high-resolution scanning transmission electron microscopy. Importantly, density functional theory studies provide unprecedented insight into the electronic structures of HEMOFs, demonstrating that the density of states in heterometallic clusters is highly sensitive to metal composition. This work dramatically advances HEMOF materials design, paving the way for further exploration of HEMs and offers new avenues for the development of multifunctional materials with tailored properties for a wide range of applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Real time lithium metal calendar aging in common battery electrolytes

Li metal anodes are highly sought after for high energy density applications in both primary commercial batteries and next-generation rechargeable batteries. In this research, Li metal electrodes are aged in coin cells for a year with electrolytes relevant to both types of batteries. The aging response is monitored via electrochemical impedance spectroscopy, and Li electrodes are characterized post-mortem. It was found that the carbonate-based electrolytes exhibit the most severe aging effects, despite the use of LiBF 4 -based carbonate electrolytes in Li/CF x Li primary batteries. Highly concentrated LiFSI electrolytes exhibit the most minimal aging effects, with only a small impedance increase with time. This is likely due to the concentrated nature of the electrolyte causing fewer solvent molecules available to react with the electrode surface. LiI-based electrolytes also show improved aging behavior both on their own and as an additive, with a similar impedance response with time as the concentrated LiFSI electrolytes. Since I − is in its most reduced state, it likely prevents further reaction and may help protect the Li electrode surface with a primarily organic solid electrolyte interphase.

25 ENERGY STORAGE↗
DOE OSTI2023

Granular metals with SiN x dielectrics

Understanding and controlling nanoscale interface phenomena, such as band bending and secondary phase formation, is crucial for electronic device optimization. In granular metal (GM) studies, where metal nanoparticles are embedded in an insulating matrix, the importance of interface phenomena is frequently neglected. Here, we demonstrate that GMs can serve as an exemplar system for evaluating the role of secondary phases at interfaces through a combination of x-ray photoemission spectroscopy (XPS) and electrical transport studies. We investigated SiN x as an alternative to more commonly used oxide-insulators, as SiN x -based GMs may enable high temperature applications when paired with refractory metals. Comparing Co-SiN x and Mo-SiN x GMs, we found that, in the tunneling-dominated insulating regime, Mo-SiN x had reduced metal-silicide formation and orders-of-magnitude lower conductivity. XPS measurements indicate that metal-silicide and metal-nitride formation are mitigatable concerns in Mo-SiN x . Given the metal-oxide formation seen in other GMs, SiN x is an appealing alternative for metals that readily oxidize. Furthermore, SiN x provides a path to metal-nitride nanostructures, potentially useful for various applications in plasmonics, optics, and sensing.

77 NANOSCIENCE AND NANOTECHNOLOGY↗