The propensity of metals to form irregular and nonplanar electrodeposits at liquid-solid interfaces has emerged as a fundamental barrier to high-energy, rechargeable batteries that use metal anodes. ...We report an epitaxial mechanism to regulate nucleation, growth, and reversibility of metal anodes. The crystallographic, surface texturing, and electrochemical criteria for reversible epitaxial electrodeposition of metals are defined and their effectiveness demonstrated by using zinc (Zn), a safe, low-cost, and energy-dense battery anode material. Graphene, with a low lattice mismatch for Zn, is shown to be effective in driving deposition of Zn with a locked crystallographic orientation relation. The resultant epitaxial Zn anodes achieve exceptional reversibility over thousands of cycles at moderate and high rates. Reversible electrochemical epitaxy of metals provides a general pathway toward energy-dense batteries with high reversibility.
Among various commercially available energy storage devices, lithium‐ion batteries (LIBs) stand out as the most compact and rapidly growing technology. This multicomponent system operates on coupled ...dynamics to reversibly store and release electricity. With the hierarchical electrode architectures inside LIBs, versatile functionality can be realized by design, while considerable difficulties remain to be solved to fully exploit the capability of each constituent. With the rapid electrification of the transportation sector and an urgent need to overhaul electric grids in the context of renewable energy penetration, demands for concomitant high energy and high power batteries are continuously increasing. Although building an ideal battery requires effort from multiple scientific and engineering aspects, it is imperative to gain insight into multiscale transport behaviors arising in both spatial and temporal dimensions, and enable their harmonic integration inside the whole battery system. In this progress report, recent research efforts on characterizing and understanding transport kinetics in LIBs are reviewed covering a broad range of electrode materials and length scales. To demonstrate the crucial role of such information in revolutionary electrode design, examples of innovative high energy/power electrodes are provided with their unique hierarchical porous architectures highlighted. To conclude, perspectives on further approaches toward advanced thick electrode designs with fast kinetics and tailored properties are discussed.
Multiscale understanding of the transport kinetics in both spatial and temporal dimensions offers great opportunities for hierarchical electrode architecture designs toward high energy/power batteries. Recent progress in understanding kinetic behaviors in lithium‐ion batteries is reviewed and favorable electrode design rationales are highlighted.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
This study develops a tunable 3D nanostructured conductive gel framework as both binder and conductive framework for lithium ion batteries. A 3D nanostructured gel framework with continuous electron ...pathways can provide hierarchical pores for ion transport and form uniform coatings on each active particle against aggregation. The hybrid gel electrodes based on a polypyrrole gel framework and Fe3O4 nanoparticles as a model system in this study demonstrate the best rate performance, the highest achieved mass ratio of active materials, and the highest achieved specific capacities when considering total electrode mass, compared to current literature. This 3D nanostructured gel‐based framework represents a powerful platform for various electrochemically active materials to enable the next‐generation high‐energy batteries.
A tunable 3D nanostructured gel framework with continuous electron pathways can provide hierarchical pores for ion transport and form uniform coatings on each active particle against aggregation. The hybrid gel electrodes based on a polypyrrole gel framework and Fe3O4 nanoparticles demonstrate one of the best rate performances and the highest achieved specific capacities when considering total electrode mass.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Controlling architecture of electrode composites is of particular importance to optimize both electronic and ionic conduction within the entire electrode and improve the dispersion of active ...particles, thus achieving the best energy delivery from a battery. Electrodes based on conventional binder systems that consist of carbon additives and nonconductive binder polymers suffer from aggregation of particles and poor physical connections, leading to decreased effective electronic and ionic conductivities. Here we developed a three-dimensional (3D) nanostructured hybrid inorganic-gel framework electrode by in situ polymerization of conductive polymer gel onto commercial lithium iron phosphate particles. This framework electrode exhibits greatly improved rate and cyclic performance because the highly conductive and hierarchically porous network of the hybrid gel framework promotes both electronic and ionic transport. In addition, both inorganic and organic components are uniformly distributed within the electrode because the polymer coating prevents active particles from aggregation, enabling full access to each particle. The robust framework further provides mechanical strength to support active electrode materials and improves the long-term electrochemical stability. The multifunctional conductive gel framework can be generalized for other high-capacity inorganic electrode materials to enable high-performance lithium ion batteries.
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IJS, KILJ, NUK, PNG, UL, UM
MgMn2O4 nanoparticles with crystallite sizes of 11 (MMO-1) and 31 nm (MMO-2) were synthesized and their magnesium-ion battery-relevant electrochemistry was investigated. MMO-1 delivered an initial ...capacity of 220 mA h g-1 (678 mW h g-1). Electrolyte water content had a profound effect on cycle retention.
Spinel transition metal oxides (TMOs) have emerged as promising anode materials for lithium-ion batteries. It has been shown that reducing their particle size to nanoscale dimensions benefits overall ...electrochemical performance. Here, we use in situ transmission electron microscopy to probe the lithiation behavior of spinel ZnFe
O
as a function of particle size. We have found that ZnFe
O
undergoes an intercalation-to-conversion reaction sequence, with the initial intercalation process being size dependent. Larger ZnFe
O
particles (40 nm) follow a two-phase intercalation reaction. In contrast, a solid-solution transformation dominates the early stages of discharge when the particle size is about 6-9 nm. Using a thermodynamic analysis, we find that the size-dependent kinetics originate from the interfacial energy between the two phases. Furthermore, the conversion reaction in both large and small particles favors {111} planes and follows a core-shell reaction mode. These results elucidate the intrinsic mechanism that permits fast reaction kinetics in smaller nanoparticles.
Charge transport is a key process that dominates battery performance, and the microstructures of the cathode, anode, and electrolyte play a central role in guiding ion and/or electron transport ...inside the battery. Rational design of key battery components with varying microstructure along the charge‐transport direction to realize optimal local charge‐transport dynamics can compensate for reaction polarization, which accelerates electrochemical reaction kinetics. Here, the principles of charge‐transport mechanisms and their decisive role in battery performance are presented, followed by a discussion of the correlation between charge‐transport regulation and battery microstructure design. The design strategies of the gradient cathodes, lithium‐metal anodes, and solid‐state electrolytes are summarized. Future directions and perspectives of gradient design are provided at the end to enable practically accessible high‐energy and high‐power‐density batteries.
Charge transport is a key process that dominates battery performance, and the microstructure of battery key components plays a central role in guiding the charge transport. By gradient design, optimal local charge‐transport dynamics can be realized and high energy/power supported. Recent processes in the gradient design strategies of cathodes, lithium‐metal anodes, and solid‐state electrolytes are presented with future research directions highlighted.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Battery systems have been developed that provide years of service for implantable medical devices. The primary systems utilize lithium metal anodes with cathode systems including iodine, manganese ...oxide, carbon monofluoride, silver vanadium oxide and hybrid cathodes. Secondary lithium ion batteries have also been developed for medical applications where the batteries are charged while remaining implanted. While the specific performance requirements of the devices vary, some general requirements are common. These include high safety, reliability and volumetric energy density, long service life, and state of discharge indication. Successful development and implementation of these battery types has helped enable implanted biomedical devices and their treatment of human disease.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
The ever‐growing needs for renewable energy demand the pursuit of batteries with higher energy/power output. A thick electrode design is considered as a promising solution for high‐energy batteries ...due to the minimized inactive material ratio at the device level. Most of the current research focuses on pushing the electrode thickness to a maximum limit; however, very few of them thoroughly analyze the effect of electrode thickness on cell‐level energy densities as well as the balance between energy and power density. Here, a realistic assessment of the combined effect of electrode thickness with other key design parameters is provided, such as active material fraction and electrode porosity, which affect the cell‐level energy/power densities of lithium–LiNi0.6Mn0.2Co0.2O2 (Li–NMC622) and lithium–sulfur (Li–S) cells as two model battery systems, is provided. Based on the state‐of‐the‐art lithium batteries, key research targets are quantified to achieve 500 Wh kg–1/800 Wh L–1 cell‐level energy densities and strategies are elaborated to simultaneously enhance energy/power output. Furthermore, the remaining challenges are highlighted toward realizing scalable high‐energy/power energy‐storage systems.
A critical assessment of the combined effect of electrode thickness with other key design parameters is provided and practical guidelines offered toward developing scalable high‐energy/power energy‐storage systems.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
•Mg-ion batteries may address future large scale mobile and stationary device needs.•Recent research on cathodes for Mg-ion is reviewed.•Chemical and structural details of the cathode materials are ...emphasized.•Particular strategies which may lead to future research initiatives are amplified.
Rechargeable magnesium-ion batteries are a promising candidate technology to address future electrical energy storage needs of large scale mobile and stationary devices, due to the high environmental abundance of magnesium metal and divalent character of magnesium ion. With the recent increase in reports discussing cathode materials for magnesium-ion batteries, it is instructive to assess recent research in order to provide inspiration for future research. This review is a summary of the different chemistries and structures of the materials developed for magnesium ion cathodes. The particular strategies which may lead to future research initiatives are amplified.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
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