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Publications (31)
Through a combination of multimodal operando, as well as and ex situ , and in situ techniques: Unravelling the intrinsic factors underlying the electrochemical activation of maricite-NaFePO 4 .
Lithium‐ion batteries (LIBs) have been the focus of research for decades owing to their superior energy storage potential and wide range of applications. However, long‐term stability issues still persist in LIB cathodes as the result of the formation of a solid electrolyte interface (SEI), structural transformations, or the loss of active cathode m...
Transition metal oxides are the promising materials as cathodes for divalent batteries with high capacity under high voltage. The major challenge is the high interaction between divalent cations and oxide host and resultant limited cation mobility. Tailoring of size, composition and crystal structure of oxides is a necessary strategy to alleviate t...
α-V2O5 has been extensively explored as a Mg2+ intercalation host with potential as a battery cathode, offering high theoretical capacities and potentials vs. Mg2+/Mg. However, large voltage hysteresis is observed with Mg insertion and extraction, introducing significant and unacceptable round-trip energy losses with cycling. Conventional interpret...
V 2 O 5 is of interest as a Mg intercalation electrode material for Mg batteries, both in its thermodynamically stable layered polymorph (α-V 2 O 5) and in its metastable tunnel structure (ζ-V 2 O 5). However, such oxide cathodes typically display poor Mg insertion/removal kinetics, with large voltage hysteresis. Herein, we report the synthesis and...
Oxides with the CaFe2O4-type structure have been predicted as suitable hosts for reactions of intercalation of light cations such as Li and Mg because of their favorable diffusion. While Li can intercalate into the Mn2O4 variant, the structure-property correlations determining function are not fully ascertained. This basic information is needed bef...
While commercial Li-ion batteries offer the highest energy densities of current rechargeable battery technologies, their energy storage limit has almost been achieved. Therefore, there is considerable interest in Mg batteries, which could offer increased energy densities in comparison to Li-ion batteries if a high-voltage electrode material, such a...
Racemates have recently received attention as nonlinear optical and piezoelectric materials. Here, a machine-learning-assisted composition space approach was applied to synthesize the missing M = Ti, Zr members of the Δ,Λ-[Cu(bpy)2(H2O)]2[MF6]2·3H2O (M = Ti, Zr, Hf; bpy = 2,2'-bipyridine) family (space group: Pna21). In each (CuO, MO2)/bpy/HF(aq) (...
The design of Mg batteries with high energy density is hindered by the lack of oxide electrodes that reversibly intercalate high levels of Mg2+ at high potential. While -V2O5 was traditionally considered one of the only moderately functional oxides as Mg battery cathode, the most recent literature indicates that electrochemical activity observed p...
Chromium oxides with the spinel structure have been predicted to be promising high voltage cathode materials in magnesium batteries. Perennial challenges involving the mobility of Mg ²⁺ and reaction kinetics can be circumvented by nano-sizing the materials in order to reduce diffusion distances, and by using elevated temperatures to overcome activa...
Chromium oxides with the spinel structure are predicted to be promising high voltage cathode materials in batteries based on the intercalation of Mg2+. Perennial challenges involving the mobility of Mg2+ and reaction kinetics can be circumvented by nano-sizing the materials in order to reduce diffusion distances, and by using elevated temperatures...
A comprehensive study on the effects of experimental parameters on the composition and size of manganese oxide nanocrystals was completed using colloidal chemistry. The reactions studied involved the thermolysis of Mn2+ acetate and Mn3+ acetylacetonate in oleylamine. Temperature was found to be the dominant factor affecting the composition and size...
Oxides undergoing reversible electrochemical cycling of Mg2+ ions would enable novel battery concepts beyond Li+, capable of storing large amounts of energy. However, materials showing this chemical reactivity are scarce. Suitable candidates require small particles to shorten transport lengths, together with chemically complex structures that pro-m...
In this report, the feasibility of reversible Ca2+ or Zn2+ intercalation into a crystalline cubic spinel Mn2O4 cathode has been investigated using electrochemical methods in an aqueous electrolyte. A combination of synchrotron XRD and XANES studies identified the partial structural transformation from a cubic to a tetragonally distorted spinel Mn3O...
Rechargeable Mg batteries are promising candidates for high energy density storage in theory, when a Mg metal anode is combined with an oxide cathode material. Despite the widely observed sluggish Mg2+ diffusion in most oxide lattices, recent first principles calculations predicted low diffusion barriers in the calcium ferrite (CF) type structures....
Li-ion batteries are the top choice in electrochemical energy storage for portable devices and mobile vehicles. However, the limited storage capacities do not quite yet meet the emerging energy demands in transportation and grid markets. Multivalent batteries based on divalent cations have attracted wide attention with high energy density/capacity...
Rechargeable Mg batteries are considered as promising candidates for energy storage. The Mg metal anode with high volumetric capacity (3833 mAh mL ⁻¹ ) and low redox potential (-2.37 V vs. S.H.E.) provides high energy density for the system, while a low price, good safety and long term utilization is maintained by the inexpensiveness, air stability...
Systematic Transmission Electron Microscopy Study Investigating Lithium and Magnesium Intercalation in Vanadium Oxide Polymorphs - Volume 23 Issue S1 - A. Mukherjee, R. F. Klie, H.D. Yoo, G. Nolis, J. Cabana, J. Andrews, S. Banerjee
The energy density of rechargeable batteries utilizing metals as anodes surpasses Li-ion batteries, which employ carbon instead. Among possible metals, magnesium represents a potential alternative to the conventional choice, lithium, in terms of storage density, safety, stability, and cost. However, a major obstacle for metal-based batteries is the...
A new family of fluorine-free solid-polymer electrolytes, for use in sodium-ion battery applications, is presented. Three novel sodium salts withdiffuse negative charges: sodium pentacyanopropenide (NaPCPI), sodium 2,3,4,5-tetracyanopirolate (NaTCP) and sodium 2,4,5-tricyanoimidazolate (NaTIM) were designed andtested in a poly(ethylene oxide) (PEO)...
Efficiently using anodes based on the deposition of light metals would be a breakthrough that would produce leaps in energy density of rechargeable batteries. Magnesium is one of such metal electrodes that are not susceptible to dendrite formation. This unique property stems from (1) the thermodynamic stability in Grignard-based electrolytes and (2...
Li-ion batteries dominate the mobile device market due their high energy density; and their application is being extended to the automotive and grid storage industries. However, charge storage limitations limit the applicability of classic Li-ion technologies into these new markets, thus triggering interest in new energy storage concepts. Multivale...
Sodium has emerged as a major contender to lithium for rechargeable battery applications. Owing to its strengths are its high abundance, low production costs and suitable redox potential (Na/Na ⁺ , E o = -2.71 V, not much less than Li/Li ⁺ , E˚=-3.05 V vs. standard hydrogen electrode). However, much like the lithium-ion battery industry, researcher...
Secondary battery technology is currently based on Li-ion technology. Assuming substantial development of electrical vehicles and/or different portable devices, the lithium sources might be not sufficient to fulfill total market demands. Strategically, it is a suitable moment to research alternatives to lithium-based energy storage technologies. A...
LiNi0.5Mn1.5O4 epitomizes the challenges imposed by high electrochemical potential reactivity on the durability of high energy density Li-ion batteries. Postsynthesis coatings have been explored as a solution to these challenges, but the fundamentals of their function have not been ascertained. To contribute to this understanding, the surface of Li...
Studies of thermal decomposition mechanism of olivine Fe1−yMnyPO4 are reported here for inert (He), oxidizing (O2) and oxidizing and moist (air) atmospheres using in situ X-ray diffraction and thermal gravimetric analysis with mass spectroscopy. The results indicate that the olivine structure is inherently stable up to at least 400 °C and y = 0.9 f...
Electrode materials for Li-ion batteries should combine electronic and ionic conductivity, structural integrity, and safe operation over thousands of lithium insertion and removal cycles. The quest for higher energy density calls for better understanding of the redox processes, charge and mass transfer occurring upon battery operation. A number of...
LiFePO4 has shown considerable promise as a cathode material in Li-ion batteries due to its stability, low toxicity and high cyclability. However, the data on thermodynamic stability of olivine phase FePO4 (o-FePO4), the delithiated form of o-LiFePO4, remains scarce and contradictory. In this work, o-FePO4 was synthesized by chemical delithiation o...