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  1. Free, publicly-accessible full text available August 22, 2023
  2. Electrochemical ion insertion into transition metal oxides forms the foundation of several energy technologies. Transition metal oxides can exhibit sluggish ion transport and/or phase-transformation kinetics during ion insertion that can limit their performance at high rates (<10 min). In this study, we investigate the role of structural water in transition metal oxides during Li + insertion using staircase potentiostatic electrochemical impedance spectroscopy (SPEIS) and electrochemical quartz crystal microbalance (EQCM) analysis of WO 3 ·H 2 O and WO 3 thin-film electrodes. Overall, the presence of structural water in WO 3 ·H 2 O improves Li + insertion kinetics compared to WO 3 and leads to a less potential-dependent insertion process. Operando electrogravimetry and 3D Bode impedance analyses of nanostructured films reveal that the presence of structural water promotes charge accommodation without significant co-insertion of solvent, leading to our hypothesis that the electrochemically induced structural transitions of WO 3 hinder the electrode response at faster timescales (<10 min). Designing layered materials with confined fluids that exhibit less structural transitions may lead to more versatile ion-insertion hosts for next-generation electrochemical technologies.
    Free, publicly-accessible full text available March 1, 2023
  3. Transition metal chalcogenide nanoparticles (NPs) are of interest for energy applications, including batteries, supercapacitors, and electrocatalysis. Many methods have been established for synthesizing Ni NPs, and conversion chemistry to form Ni oxide and phosphides from template Ni NPs is well-understood. Sulfidation and selenidation of Ni NPs have been much less explored, however. We report a method for the conversion of Ni template NPs into sulfide and selenide product NPs using elemental sulfur, 1-hexadecanthiol, thiourea, trioctylphosphine sulfide, elemental selenium, and selenourea. While maintaining mole ratios of 2 mmol sulfur/selenium precursor: mmol Ni, products with phases of Ni3S2, Ni9S8, NiS, NiSO4·6H2O, Ni3S4, Ni3Se2, and NiSe have been obtained. The products have voids that form through the Kirkendall effect during interdiffusion. Trends relating the chemical properties of the precursors to the phases of the products have been identified. While some precursors contained phosphorus, there was no significant incorporation of phosphorus in any of the products. An increase of the NP size during sulfidation and selenidation is consistent with ripening. The application of Ni sulfide and selenide NPs as electrocatalysts for the hydrogen evolution reaction is also demonstrated.
  4. Through diversity of composition, sequence, and interfacial structure, hybrid materials greatly expand the palette of materials available to access novel functionality. The NSF Division of Materials Research recently supported a workshop (October 17–18, 2019) aiming to (1) identify fundamental questions and potential solutions common to multiple disciplines within the hybrid materials community; (2) initiate interfield collaborations between hybrid materials researchers; and (3) raise awareness in the wider community about experimental toolsets, simulation capabilities, and shared facilities that can accelerate this research. This article reports on the outcomes of the workshop as a basis for cross-community discussion. The interdisciplinary challenges and opportunities are presented, and followed with a discussion of current areas of progress in subdisciplines including hybrid synthesis, functional surfaces, and functional interfaces.