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Electrical conductivity and acoustic loss Q−1 of single crystalline Li(Nb,Ta)O3 solid solutions (LNT) are studied as a function of temperature by means of impedance spectroscopy and resonant piezoelectric spectroscopy, respectively. For this purpose, bulk acoustic wave resonators with two different Nb/Ta ratios are investigated. The obtained results are compared to those previously reported for congruent LiNbO3. The temperature dependent electrical conductivity of LNT and LiNbO3 show similar behavior in air at high temperatures from 400 to 700 °C. Therefore, it is concluded that the dominant transport mechanism in LNT is the same as in LN, which is the Li transport via Li vacancies. Further, it is shown that losses in LNT strongly increase above about 500 °C, which is interpreted to originate from conductivity-related relaxation mechanism. Finally, it is shown that LNT bulk acoustic resonators exhibit significantly lower loss, comparing to that of LiNbO3.

Amorphous silicon is a promising high-capacity anode material for application in lithium-ion batteries. However, a huge drawback of the material is that the large capacity losses taking place during cycling lead to an unstable performance. In this study we investigate the capacity losses occurring during galvanostatic lithiation of amorphous silicon thin film electrodes by in-situ neutron reflectometry experiments for the first ten cycles. As determined from the analysis of the neutron scattering length density and of the film thickness, the capacity losses are due to irreversible storage of lithium in the electrode. The amount of stored lithium increases during cycling to 20% of the maximum theoretical capacity after the 10th cycle. Possible explanations are discussed.

Operando neutron reflectometry measurements were carried out to study the insertion of lithium into amorphous silicon film electrodes during cyclic voltammetry CV experiments at a scan rate of 0.01 mV s amp; 8722;1. The experiments allow mapping of regions where significant amounts of Li are incorporated released from the electrode and correlation of the results to modifications of characteristic peaks in the CV curve. High volume changes up to 390 accompanied by corresponding modifications of the neutron scattering length density which is a measure of the average Li fraction present in the electrode are observed during electrochemical cycling for potentials below 0.3 V lithiation and above 0.2 V delithiation , leading to a hysteretic behaviour. This is attributed to result from mechanical stress as suggested in the literature. Formation and modification of a surface layer associated with the solid electrolyte interphase SEI were observed during cycling. Within the first lithiation cycle the SEI grows to 120 for potentials below 0.5 V. Afterwards a reversible and stable modification of the SEI between 70 delithiated state and 120 lithiated state takes place

The effect of cold-rolling on structure, thermal stability, and compressive and tensile mechanical properties of the Zr52.5Ti5Cu18Ni14.5Al10 bulk metallic glass has been investigated. The results reveal that cold-rolling does not influence the thermal stability of the material. However, the small plastic deformation induced by cold-rolling is very effective for improving the room temperature plastic strain of the glass: the compressive plastic strain increases from 1.1% for the as-cast material to 2.6% for the cold-rolled sample and the tensile ductility increases from 0% for the as-cast glass to 0.8% for the cold-rolled sample. Hardness measurements indicate that cold rolling creates a heterogeneous microstructure consisting of hard and soft regions. Most likely, the soft regions are preferred locations for shear band formation and propagation, whereas the hard regions may act as obstacles for shear band propagation, effectively limiting shear bands from propagating catastrophically and, consequently, enhancing the room temperature plastic deformation of the glass.

Neutron reflectometry is used to study in situ the intercalation of lithium into amorphous silicon electrodes. The experiments are done using a closed three-electrode electrochemical cell setup. As a working electrode, an about 40 nm thick amorphous silicon layer is used that is deposited on a 1 cm thick quartz substrate coated with palladium as a current collector. The counter electrode and the reference electrode are made of lithium metal. Propylene carbonate with 1 M LiClO4 is used as an electrolyte. The utility of the cell is demonstrated during neutron reflectometry measurements where Li is intercalated at a constant current of 100 μA (7.8 μA cm(-2)) for different time steps. The results show (a) that the change in Li content in amorphous silicon and the corresponding volume expansion can be monitored, (b) that the formation of the solid electrolyte interphase becomes visible and (c) that an irreversible capacity loss is present.

Experiments on self-diffusion in amorphous silicon between 400 and 500 °C are presented, which were carried out by neutron reflectometry in combination with 29Si/natSi isotope multilayers. Short range diffusion is detected on a length scale of about 2 nm, while long range diffusion is absent. Diffusivities are in the order of 10−19–10−20 m2/s and decrease with increasing annealing time, reaching an undetectable low value for long annealing times. This behavior is strongly correlated to structural relaxation and can be explained as a result of point defect annihilation. Diffusivities for short annealing times of 60 s follow the Arrhenius law with an activation enthalpy of (0.74 ± 0.21) eV, which is interpreted as the activation enthalpy of Si migration.

Kinetic processes and interface phenomena at electrodes during charging and discharging cycles play a key role for optimization of lithium-ion batteries (e.g. for charging times and power density). In order to study lithium insertion/de-insertion into electrodes and the underlying mechanisms, we applied neutron reflectometry as a non-destructive analysis technique. This method allows to study lithiation in-operando during cell operation. As negative electrode material, silicon is used a promising candidate for future Li-ion battery applications due to its high theoretical specific capacity of about 4 Ah/g. The experiments are done using a three electrode electrochemical cell setup with a layered nanometer-sized amorphous silicon anode. The working electrode is deposited by magnetron sputtering on a quartz block covered by a current collector. Counter and reference electrode are made of pure lithium. A liquid electrolyte is used together with a housing made of high density polyethylene. The experiments allow to monitor the modification of Li content and the corresponding volume expansion/contraction of the electrode during lithiation on the nanometer scale. The measurements indicate that during galvanostatic charging Li incorporation takes place in form of a process, where a moving LixSi phase boundary plays an important role. Possible lithiation mechanisms are discussed. Neutron reflectometry measurements during cyclic voltammetry allow to identify regions (U/I characteristics) where considerable lithium incorporation takes place and where not. For comparison, experiments on the lithiation of massive crystalline silicon blocks are shown. B. Jerliu et al. Phys. Chem. Chem. Phys., 15, 7777, (2013)