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Creators/Authors contains: "Neale, Zachary"

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  1. Iron hexacyanoferrate (FeHCF) particles were synthesized at room temperature with ethylenediaminetetraacetic acid (EDTA) at varying pH. The presence of EDTA produced faceted particles and increasing synthesis pH resulted in slower reaction kinetics and larger particles with lower water content and fewer anion vacancies determined by TGA and Mössbauer spectroscopy. Electrochemical testing of sodium metal half cells revealed higher capacity in FeHCF particles grown at lower pH with EDTA, obtaining a maximum discharge capacity of 151 mA h g −1 with 79% capacity retention after 100 cycles at 100 mA g −1 and a rate capability of 122 mA h g −1 at 3.2 A g −1 . In contrast, particles grown at higher pH had stunted low-spin Fe redox activity but with improved long-term cyclic stability. These findings demonstrate that small changes in synthesis pH can greatly affect the growth and electrochemical properties of FeHCF when using a pH sensitive chelating agent such as EDTA. 
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  2. Hydrated vanadates are promising layered cathodes for aqueous zinc-ion batteries owing to their specific capacity as high as 400 mA h g −1 ; however, the structural instability causes serious cycling degradation through repeated intercalation/deintercalation reactions. This study reveals the chemically inserted Mn( ii ) cations act as structural pillars, expand the interplanar spacing, connect the adjacent layers and partially reduce pentavalent vanadium cations to tetravalent. The expanded interplanar spacing to 12.9 Å reduces electrostatic interactions, and transition metal cations collectively promote and catalyze fast and more zinc ion intercalation at higher discharge current densities with much enhanced reversibility and cycling stability. Manganese expanded hydrated vanadate (MnVO) delivers a specific capacity of 415 mA h g −1 at a current density of 50 mA g −1 and 260 mA h g −1 at 4 A g −1 with a capacity retention of 92% over 2000 cycles. The energy efficiency increases from 41% for hydrated vanadium pentoxide (VOH) to 70% for MnVO at 4 A g −1 and the open circuit voltage remains at 85% of the cutoff voltage in the MnVO battery on the shelf after 50 days. Expanded hydrated vanadate with other transition metal cations for high-performance aqueous zinc-ion batteries is also obtained, suggesting it is a general strategy for exploiting high-performance cathodes for multi-valent ion batteries. 
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  3. Abstract The ever‐increasing demand for clean sustainable energy has driven tremendous worldwide investment in the design and exploration of new active materials for energy conversion and energy‐storage devices. Tailoring the surfaces of and interfaces between different materials is one of the surest and best studied paths to enable high‐energy‐density batteries and high‐efficiency solar cells. Metal‐halide perovskite solar cells (PSCs) are one of the most promising photovoltaic materials due to their unprecedented development, with their record power conversion efficiency (PCE) rocketing beyond 25% in less than 10 years. Such progress is achieved largely through the control of crystallinity and surface/interface defects. Rechargeable batteries (RBs) reversibly convert electrical and chemical potential energy through redox reactions at the interfaces between the electrodes and electrolyte. The (electro)chemical and optoelectronic compatibility between active components are essential design considerations to optimize power conversion and energy storage performance. A focused discussion and critical analysis on the formation and functions of the interfaces and interphases of the active materials in these devices is provided, and prospective strategies used to overcome current challenges are described. These strategies revolve around manipulating the chemical compositions, defects, stability, and passivation of the various interfaces of RBs and PSCs. 
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