John B. Goodenough

High Resolution Image Download MS PowerPoint Slide Layered Na x MO 2 sodium oxide positive electrode materials have experienced renewed interest owing to the current commercial attention on sodium-ion batteries. Although there are many attractive qualities of these materials, they suffer from serious shortcomings owing to Na + ordering and transition-metal layer gliding that cause a plethora of voltage plateaus during cycling. The P2-layered Na 2+ x Ni 2– x /2 TeO 6 (0 ≤ x ≤ 0.5) system provides a framework for investigating the effect of dual Na + substitution into the sodium layer and the transition-metal layer of the structure and its effects on the electrochemical properties of the materials. A careful investigation into the synthesis and properties of these materials reveals that the sodium content used during material preparation has a drastic effect on the composition and electrochemical profile of these materials. The sodium substitution disrupts ordering within the transition-metal layer, thereby disrupting Na + ordering in the adjacent sodium layers. Beyond a critical sodium concentration, the layer stacking shifts, and all voltage plateaus of the P2-Na 2 Ni 2 TeO 6 material are no longer observed at 4.4 V versus Na + /Na. These results also question the common belief that additional sodium precursor is required when preparing layered sodium oxide cathodes, providing new guidelines for material synthesis and characterization.

A new perovskite KOsO_{3} has been stabilized under high-pressure and high-temperature conditions. It is cubic at 500 K (Pm-3m) and undergoes subsequent phase transitions to tetragonal at 320 K (P4/mmm) and rhombohedral (R-3m) at 230 K as shown from refining synchrotron x-ray powder diffraction (SXRD) data. The larger orbital overlap integral and the extended wave function of 5d electrons in the perovskite KOsO_{3} allow to explore physics from the regime where Mott and Hund's rule couplings dominate to the state where the multiple interactions are on equal footing. We demonstrate an exotic magnetic ordering phase found by neutron powder diffraction along with physical properties via a suite of measurements including magnetic and transport properties, differential scanning calorimetry, and specific heat, which provide comprehensive information for a system at the crossover from localized to itinerant electronic behavior.

A new perovskite KOsO3 has been stabilized under high-pressure and high temperature conditions. It is cubic at 500 K (Pm-3m) and undergoes subsequent phase transitions to tetragonal at 320 K (P4/mmm) and rhombohedral (R-3m) at 230 K as shown from refining synchrotron X-ray powder diffraction (SXRD) data. The larger orbital overlap integral and the extended wavefunction of 5d electrons in the perovskite KOsO3 allow to explore physics from the regime where Mott and Hund's rule couplings dominate to the state where the multiple interactions are on equal footing. We demonstrate an exotic magnetic ordering phase found by neutron powder diffraction along with physical properties via a suite of measurements including magnetic and transport properties, differential scanning calorimetry, and specific heat, which provide comprehensive information for a system at the crossover from localized to itinerant electronic behavior.

In contrast to the Mott transition found in $R\mathrm{Ni}{\mathrm{O}}_{3}$ ($R$= rare earths), the metal-insulator transition temperature in the perovskite $\mathrm{NaOs}{\mathrm{O}}_{3}$ is not sensitive to pressure. The peculiarity may be correlated to how the crystal structure of $\mathrm{NaOs}{\mathrm{O}}_{3}$ responds to high pressure, which has been rarely studied so far. The pressure-induced bond-length shrinking can increase the orbital overlap integral and therefore the electron bandwidth. However, in the orthorhombic perovskite structure, the pressure-induced bending in the bond angle Os-O-Os may compensate for the bandwidth broadening due to the bond-length shrinking in some circumstances. A recent structural study on polycrystalline $\mathrm{NaOs}{\mathrm{O}}_{3}$ indicated that orthorhombic distortion is enlarged under high pressure. But, how the local structure changes under pressure remains unknown. Moreover, a highly unusual phase transition from the orthorhombic phase (Pbnm) to a polar phase ($Pbn{2}_{1}$) occurs at around 18 GPa [Sereika et al., npj Quantum Mater. 5, 66 (2020)]. Motivated by these concerns, we have done a more comprehensive structural study on $\mathrm{NaOs}{\mathrm{O}}_{3}$ using single-crystal diffraction with synchrotron radiation at high pressures up to 41 GPa. Diffraction patterns over the entire pressure range can be refined well with the Pbnm structural model. Moreover, the refinement results reveal in detail how the local structures change under pressure corresponding to the enhanced orthorhombic distortion from the lattice parameters. We have carried out a systematic study for understanding the pressure effect on the orthorhombic perovskites in the context of the influences of the charge distributions in the $AB{\mathrm{O}}_{3}$ formula, i.e., ${A}^{3+}{B}^{3+}{\mathrm{O}}_{3}$, ${A}^{2+}{B}^{4+}{\mathrm{O}}_{3}$, and ${A}^{1+}{B}^{5+}{\mathrm{O}}_{3}$ and the $B$-site cations from the $3d$ to the $4d$ and $5d$ row of elements. To fulfill this purpose, we have revisited two families of $3d$ perovskites: $R\mathrm{Cr}{\mathrm{O}}_{3}$ and $R\mathrm{Fe}{\mathrm{O}}_{3}$.

Abstract Employing high voltage cobalt‐free spinel LiNi 0.5 Mn 1.5 O 4 (LNMO) as a cathode is promising for high energy density and cost‐effectiveness, but it has challenges in all‐solid‐state batteries (ASSBs). Here, it is revealed that the limitation of lithium argyrodite sulfide solid electrolyte (Li 6 PS 5 Cl) with the LNMO cathode is due to the intrinsic chemical incompatibility and poor oxidative stability. Through a careful analysis of the interphase of LNMO, it is elucidated that even the halide solid electrolyte (Li 3 InCl 6 ) with high oxidative stability can be decomposed to form resistive interphase layers with LNMO in ASSBs. Interestingly, with Fe‐doping and a Li 3 PO 4 protective layer coating, LNMO with Li 3 InCl 6 displays stable cycle performance with a stabilized interphase at a high voltage (≈4.7 V) in ASSBs. The enhanced interfacial stability with the extended electrochemical stability window through doping and coating enables high electrochemical stability with LNMO in ASSBs. This work provides guidance for employing high‐voltage cathodes in ASSBs and highlights the importance of stable interphases to enable stable cycling in ASSBs.

Abstract All‐solid‐state lithium‐metal batteries offer higher energy density and safety than lithium‐ion batteries, but their practical applications have been pushed back by the sluggish Li + transport, unstable electrolyte/electrode interface, and/or difficult processing of their solid‐state electrolytes. Li + ‐conducting composite polymer electrolytes (CPEs) consisting of sub‐micron particles of an oxide solid‐state electrolyte (OSSE) dispersed in a solid, flexible polymer electrolyte (SPE) have shown promises to alleviate the low Li + conductivity of SPE, and the high rigidity and large interfacial impedance of OSSEs. Solution casting has been by far the most widely used procedure for the preparation of CPEs in research laboratories; however, this method imposes several drawbacks including particle aggregation and settlement during a long‐term solvent evaporation step, excessive use of organic solvents, slow production time, and mechanical issues associated with handling of ultra‐thin films of CPEs (<50 µm). To address these challenges, an electrophoretic deposition (EPD) method is developed to in situ deposit ultra‐thin CPEs on lithium‐iron‐phosphate (LFP) cathodes within just a few minutes. EPD‐prepared CPEs have shown better electrochemical performance in the lithium‐metal battery than those CPEs prepared by solution casting due to a better dispersion of OSSE within the SPE matrix and improved CPE contact with LFP cathodes.

An assurance case for a critical system is valid for that system at a particular point in time, such as when the system is delivered to a certification authority for review. The argument is structured around evidence that exists at that point in time. However, modern assurance cases are rarely one-off exercises. More information might become available (e.g., field data) that could strengthen (or weaken) the validity of the case. This paper proposes the notion of incremental assurance wherein the assurance case structure includes both the currently available evidence and a plan for incrementally increasing confidence in the system as additional or higher quality evidence becomes available. Such evidence is needed to further reduce doubts engineers or reviewers might have. This paper formalizes the idea of incremental assurance through an argumentation pattern. The concept of incremental assurance is demonstrated by applying the pattern to part of a safety assurance case for an air traffic control system.

A rechargeable battery cell has an organic-liquid electrolyte contacting a dendrite free alkali-metal anode. The alkali-metal anode may be a liquid at the operating temperature that is immobilized by absorption into a porous membrane. The alkali-metal anode may be a solid that wets a porous-membrane separator, where the contact between the solid alkali-metal anode and the liquid electrolyte is at micropores or nanopores in the porous-membrane separator. The use of a dendrite-free solid lithium cell was demonstrated in a symmetric cell with a porous cellulose-based separator membrane. A K+-ion rechargeable cell was demonstrated with a liquid K—Na alloy anode immobilized in a porous carbon membrane using an organic-liquid electrolyte with a Celgard® or glass-fiber separator.

The present invention includes an apparatus and method of making and using a composition that includes the replacement of electrochemically inactive additives with a conductive and electrochemically active polymer that is attached so as to make an electrical contract to the redox couples of the electrochemically active oxide particles into/from which Lithium is reversibly inserted/extracted in a battery discharge/charge cycle.

Abstract A solid‐state battery with a lithium‐metal anode and a garnet‐type solid electrolyte has been widely regarded as one of the most promising solutions to boost the safety and energy density of current lithium‐ion batteries. However, lithiophobic property of garnet‐type solid electrolytes hinders the establishment of a good physical contact with lithium metal, bringing about a large lithium/garnet interfacial resistance that has remained as the greatest issue facing their practical application in solid‐state batteries. Herein, a melt‐quenching approach is developed by which varieties of interfacial modification layers based on metal alloys can be coated uniformly on the surface of the garnet. It is demonstrated that with an ultrathin, lithiophilic AgSn 0.6 Bi 0.4 O x coating the interfacial resistance can be eliminated, and a dendrite‐free lithium plating and stripping on the lithium/garnet interface can be achieved at a high current density of 20 mA cm −2 . The results reveal that the uniform coating on the garnet surface and the facile lithium diffusion through the coating layer are two major reasons for the excellent electrochemical performances. The all‐solid‐state full cell consisting of the surface modified garnet‐type solid electrolyte with a LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode and a lithium–metal anode maintains 86% of its initial capacity after 1000 stable cycles at 1 C.