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Garnet-type Li7La3Zr2O12 (LLZO) is a promising solid electrolyte for all-solid-state batteries due to its structural stability and high Li+ ionic conductivity, but high-purity LLZO crystallizes in a low-conductivity tetragonal phase at room temperature (RT). Al doping stabilizes the cubic structure, yet its impact on Li+ migration is not fully understood. Using Li6.25La3Zr2Al0.25O12 (LLZAO) as a model, we conducted temperature-dependent neutron powder diffraction (NPD), neutron pair distribution function (nPDF), and density-functional theory (DFT) computations. NPD results, supported by nPDF, show Li+ ions at 24d and 96h sites, excluding 48g. Al at 24d adjusts the distribution of Li, improving ionic conductivity near RT. Maximum Entropy Method analyses indicate a temperature-driven 3D Li diffusion pathway of 24d-96h-96h-24d channels, confirmed by DFT. This work will enhance the understanding of Li diffusion and the optimization of ionic conductivity in garnet-type solid electrolytes. [ABSTRACT FROM AUTHOR]

High‐voltage ultrahigh‐Ni cathodes (LiNixCoyMn1−x−yO2, x≥0.9) can significantly enhance the energy density and cost‐effectiveness of Li‐ion batteries beyond current levels. However, severe Li−Ni antisite defects and their undetermined dynamic evolutions during high‐voltage cycling limit the further development of these ultrahigh‐Ni cathodes. In this study, we quantify the dynamic evolutions of the Li−Ni antisite defect using operando neutron diffraction and reveal its coupling relationship with anionic redox, another critical challenge restricting ultrahigh‐Ni cathodes. We detect a clear Ni migration coupled with an unstable oxygen lattice, which accompanies the oxidation of oxygen anions at high voltages. Based on these findings, we propose that minimized Li−Ni antisite defects and controlled Ni migrations are essential for achieving stable high‐voltage cycling structures in ultrahigh‐Ni cathodes. This is further demonstrated by the optimized ultrahigh‐Ni cathode, where reduced dynamic evolutions of the Li−Ni antisite defect effectively inhibit the anionic redox, enhancing the 4.5 V cycling stability. [ABSTRACT FROM AUTHOR]

By using temperature-dependent neutron powder diffraction combined with maximum entropy method analysis, a previously unreported Li lattice site was discovered in the argyrodite Li6PS5Cl solid-state electrolyte. This new finding enables a more complete description of the Li diffusion model in argyrodites, providing structural guidance for designing novel high-conductivity solid-state electrolytes. [ABSTRACT FROM AUTHOR]

Nanostructuring, structure distortion, and/or disorder are the main manipulation techniques to reduce the lattice thermal conductivity and improve the figure of merit of thermoelectric materials. A single-phase α-MgAgSb sample, MgAg0.97Sb0.99, with high thermoelectric performance in near room temperature region was synthesized through a high-energy ball milling with a hot-pressing method. Here, we report the average grain size of 24–28 nm and the accurate structure distortion, which are characterized by high-resolution neutron diffraction and synchrotron x-ray diffraction with Rietveld refinement data analysis. Both the small grain size and the structure distortion have a contribution to the low lattice thermal conductivity in MgAg0.97Sb0.99. [ABSTRACT FROM AUTHOR]

In layered LiNi x Mn y Co z O 2 cathode material for lithium-ion batteries, the spins of transition metal (TM) ions construct a two-dimensional triangular networks, which can be considered as a simple case of geometrical frustration. By performing neutron powder diffraction experiments and magnetization measurements, we find that long-range magnetic order cannot be established in LiNi x Mn y Co z O 2 even at low temperature of 3 K. Remarkably, the frustration parameters of these compounds are estimated to be larger than 30, indicating the existence of strongly frustrated magnetic interactions between spins of TM ions. As frustration will inevitably give rise to lattice instability, the formation of Li/Ni exchange in LiNi x Mn y Co z O 2 will help to partially relieve the degeneracy of the frustrated magnetic lattice by forming a stable antiferromagnetic state in hexagonal sublattice with nonmagnetic ions located in centers of the hexagons. Moreover, Li/Ni exchange will introduce 180° superexchange interaction, which further relieves the magnetic frustration through bringing in new exchange paths. Thus, the variation of Li/Ni exchange ratio vs. TM mole fraction in LiNi x Mn y Co z O 2 with different compositions can be well understood and predicted in terms of magnetic frustration and superexchange interactions. This provides a unique viewpoint to study the Li/Ni ions exchange in layered Li(Ni x Mn y Co z )O 2 cathode materials. [ABSTRACT FROM AUTHOR]

Li2MnO3 is the parent compound of the well-studied Li-rich Mn-based cathode materials xLi2MnO3·(1- x)LiMO2 for high-energy-density Li-ion batteries. Li2MnO3 has a very high theoretical capacity of 458 mA h g−1 for extracting 2 Li. However, the delithiation and lithiation behaviors and the corresponding structure evolution mechanism in both Li2MnO3 and Li-rich Mn-based cathode materials are still not very clear. In this research, the atomic structures of Li2MnO3 before and after partial delithiation and re-lithiation are observed with spherical aberration-corrected scanning transmission electron microscopy (STEM). All atoms in Li2MnO3 can be visualized directly in annular bright-field images. It is confirmed accordingly that the lithium can be extracted from the LiMn2 planes and some manganese atoms can migrate into the Li layer after electrochemical delithiation. In addition, the manganese atoms can move reversibly in the (001) plane when ca. 18.6% lithium is extracted and 12.4% lithium is re-inserted. LiMnO2 domains are also observed in some areas in Li1.63MnO3 at the first cycle. As for the position and occupancy of oxygen, no significant difference is found between Li1.63MnO3 and Li2MnO3. [ABSTRACT FROM AUTHOR]

Magnetic structure of Pr6Fe13Ge at room temperature has been investigated by magnetic measurement, Mössbauer effect and neutron diffraction. Magnetic atoms are closely packed up and down the mirror planes at z = 0 and 1/2 and separated by the non-magnetic atoms located on the planes at z= 1/4 and 3/4, which constructs an M/NM/M sandwich structure (M: magnetic, NM: non-magnetic). The intralayer magnetic moments couple ferromagnetically and are out of ab plane at a small angle so as to form a component along c-axis. The interlayer coupling is antiferromagnetic for the ab component while ferromagnetic for the c component. [ABSTRACT FROM AUTHOR]

Garnet-type Li7La3Zr2O12 (LLZO) is a promising solid electrolyte for all-solid-state batteries due to its structural stability and high Li+ ionic conductivity, but high-purity LLZO crystallizes in a low-conductivity tetragonal phase at room temperature (RT). Al doping stabilizes the cubic structure, yet its impact on Li+ migration is not fully understood. Using Li6.25La3Zr2Al0.25O12 (LLZAO) as a model, we conducted temperature-dependent neutron powder diffraction (NPD), neutron pair distribution function (nPDF), and density-functional theory (DFT) computations. NPD results, supported by nPDF, show Li+ ions at 24d and 96h sites, excluding 48g. Al at 24d adjusts the distribution of Li, improving ionic conductivity near RT. Maximum Entropy Method analyses indicate a temperature-driven 3D Li diffusion pathway of 24d-96h-96h-24d channels, confirmed by DFT. This work will enhance the understanding of Li diffusion and the optimization of ionic conductivity in garnet-type solid electrolytes. [ABSTRACT FROM AUTHOR]

The T0 chopper has the ability to remove the fast neutrons and high-energy gamma rays emitted at time zero of each pulse cycle. The multi-physics instrument of the China Spallation Neutron Source requires high epithermal neutron flux to obtain large momentum transfer, and the traditional single T0 chopper is a disadvantage for the transmission of epithermal neutrons in the long focusing guide. To solve this problem, the two counter-rotating T0 chopper design is proposed that can greatly improve the transmission efficiency of epithermal neutrons. The results of the beam experiment show that compared with the single T0 chopper operating at 50 Hz, the two counter-rotating T0 choppers at the same speed significantly improves the transmission efficiency of epithermal neutrons (especially the shorter wavelength neutrons). For example, when the two blades partially overlap, the transmission efficiencies of 0.05 Å, 0.1 Å, and 0.2 Å wavelength neutrons are increased by 9.4, 4.7, and 4.6 times, respectively, which fully proves that the two counter-rotating T0 chopper design is reasonable, and the experimental results are in line with expectations. The design and application of two counter-rotating T0 choppers at the China Spallation Neutron Source is the first example of this in the world and can be applied to neutron spectrometers with high epithermal neutron flux requirements, and can also be extended to fields such as the energy selection of high-energy particles. [ABSTRACT FROM AUTHOR]