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The surface treatment for a polymer‐ceramic composite is additionally performed in advanced material industries. To prepare the composite without a surface treatment, the simplest way to manufacture an advanced ceramic‐particle is devised. The method is the formation of a nanocrystalline composite layer through the simple liquid‐phase sintering. Using magnesia (MgO) which shows hydrophilicity, a nanocrystalline surface layer is realized by liquid‐phase sintering. The amorphous matrix of nanocrystalline composite layer makes MgO hydrophobic and ensures miscibility with polymers, and the nanocrystalline MgO ensures high thermal conductivity. In addition, the liquid phase removes the open pores and makes the surface morphology smooth MgO with smooth surface (MgO‐SM). Thermal interface materials (TIM) prepared with MgO‐SM and epoxy show a high thermal conductivity of ≈7.5 W m−1K−1, which is significantly higher than 4.5 W m−1K−1 of pure MgO TIM. Consequently, the formation process of a nanocrystalline surface layer utilizing simple liquid‐phase sintering is proposed as a fabrication method for a next‐generation ceramic‐filler. In addition, it is fundamentally identified that the thermal conductivity of MgO depends on the Mg deficiency, and therefore a poly‐crystal MgO‐SM (produced at a low temperature) has a higher thermal conductivity than a single‐crystal MgO (produced at a high temperature). [ABSTRACT FROM AUTHOR]

The oxygen stacking of O3‐type layered sodium transition metal oxides (O3‐NaTMO2) changes dynamically upon topotactic Na extraction and reinsertion. While the phase transition from octahedral to prismatic Na coordination that occurs at intermediate desodiation by transition metal slab gliding is well understood, the structural evolution at high desodiation, crucial to achieve high reversible capacity, remains mostly uncharted. In this work, the phase transitions of O3‐type layered NaTMO2 at high voltage are investigated by combining experimental and computational approaches. An OP2‐type phase that consists of alternating octahedral and prismatic Na layers is directly observed by in situ X‐ray diffraction and high‐resolution scanning transmission electron microscopy. The origin of this peculiar phase is explained by atomic interactions involving Jahn–Teller active Fe4+ and distortion tolerant Ti4+ that stabilize the local Na environment. The path‐dependent desodiation and resodiation pathways are also rationalized in this material through the different kinetics of the prismatic and octahedral layers, presenting a comprehensive picture about the structural stability of the layered materials upon Na intercalation. [ABSTRACT FROM AUTHOR]

Abstract: The exploration of high‐energy‐density cathode materials is vital to the practical use of K‐ion batteries. Layered K‐metal oxides have too high a voltage slope due to their large K+–K+ interaction, resulting in low specific capacity and average voltage. In contrast, the 3D arrangement of K+, with polyanions separating them, reduces the strength of the effective K+‐K+ repulsion, which in turn increases specific capacity and voltage. Here, stoichiometric KVPO4F for use as a high‐energy‐density K‐ion cathode is developed. The KVPO4F cathode delivers a reversible capacity of ≈105 mAh g−1 with an average voltage of ≈4.3 V (vs K/K+), resulting in a gravimetric energy density of ≈450 Wh kg−1. During electrochemical cycling, the KxVPO4F cathode goes through various intermediate phases at x = 0.75, 0.625, and 0.5 upon K extraction and reinsertion, as determined by ex situ X‐ray diffraction characterization and ab initio calculations. This work further explains the role of oxygen substitution in KVPO4+xF1−x: the oxygenation of KVPO4F leads to an anion‐disordered structure which prevents the formation of K+/vacancy orderings without electrochemical plateaus and hence to a smoother voltage profile. [ABSTRACT FROM AUTHOR]

Abstract: The development of rechargeable batteries using K ions as charge carriers has recently attracted considerable attention in the search for cost‐effective and large‐scale energy storage systems. In light of this trend, various materials for positive and negative electrodes are proposed and evaluated for application in K‐ion batteries. Here, a comprehensive review of ongoing materials research on nonaqueous K‐ion batteries is offered. Information on the status of new materials discovery and insights to help understand the K‐storage mechanisms are provided. In addition, strategies to enhance the electrochemical properties of K‐ion batteries and computational approaches to better understand their thermodynamic properties are included. Finally, K‐ion batteries are compared to competing Li and Na systems and pragmatic opportunities and future research directions are discussed. [ABSTRACT FROM AUTHOR]

In materials containing 1D lithium diffusion channels, cation disorder can strongly affect lithium intercalation processes. This work presents a model to explain the unusual transport properties of monoclinic LiMnBO3, a material determined by scanning electron microscopy and synchrotron X-ray diffraction to contain a wide particle size distribution and Mn/Li antisite disorder. First-principles calculations indicate that Mn occupying Li sites obstruct the 1D lithium diffusion channel along the [001] direction. While channel blockage by the antisites significantly lowers Li mobility in large particles, Li kinetics in small particles and particle surfaces are found to be less sensitive to the presence of antisite disorder. Thus, in an electrode containing a large particle size distribution, smaller particles have higher Li mobility, and the measured Li diffusivity as determined by potentiostatic intermittent titration test varies as a function of particle size. The Li capacity in monoclinic LiMnBO3 is kinetically controlled by the fraction of large particles with antisite disorder, but is not intrinsically limited. These results strongly suggest that particle nanosizing will significantly enhance the electrochemical performance of LiMnBO3. [ABSTRACT FROM AUTHOR]

In materials containing 1D lithium diffusion channels, cation disorder can strongly affect lithium intercalation processes. This work presents a model to explain the unusual transport properties of monoclinic LiMnBO3, a material determined by scanning electron microscopy and synchrotron X-ray diffraction to contain a wide particle size distribution and Mn/Li antisite disorder. First-principles calculations indicate that Mn occupying Li sites obstruct the 1D lithium diffusion channel along the [001] direction. While channel blockage by the antisites significantly lowers Li mobility in large particles, Li kinetics in small particles and particle surfaces are found to be less sensitive to the presence of antisite disorder. Thus, in an electrode containing a large particle size distribution, smaller particles have higher Li mobility, and the measured Li diffusivity as determined by potentiostatic intermittent titration test varies as a function of particle size. The Li capacity in monoclinic LiMnBO3 is kinetically controlled by the fraction of large particles with antisite disorder, but is not intrinsically limited. These results strongly suggest that particle nanosizing will significantly enhance the electrochemical performance of LiMnBO3. [ABSTRACT FROM AUTHOR]

Flexible energy‐storage devices increasingly attract attention owing to their advantages of providing lightweight, portable, wearable, or implantable capabilities. Many efforts are made to explore the structures and fabrication processes of flexible energy‐storage devices for commercialization. Here, the most recent advances in flexible energy‐storage devices based on graphene, graphene oxide (GO), and carbon nanotubes (CNTs), are described, including flexible supercapacitors and batteries. First, properties, synthesis methods, and possible applications of those carbon‐based materials are described. Then, the development of carbon‐nanotube‐based flexible supercapacitors, graphene/graphene‐oxide‐based flexible supercapacitors, and graphene‐ and carbon‐nanotube‐based flexible battery electrodes are discussed. Finally, the future trends and perspectives in the development of flexible energy‐storage devices are highlighted. [ABSTRACT FROM AUTHOR]

Cubic Na3PSe4 as a solid-state electrolyte for room temperature Na-ion batteries is prepared by solid state reaction of stoichiometric amounts of Na2Se, red P, and Se under Ar (BN tube, 300 °C, 12 h). [ABSTRACT FROM AUTHOR]