Data of physical and electrochemical characteristics of calendered NMC622 electrodes and lithium-ion cells at pilot-plant battery manufacturing.

The data reported here was prepared to study the effects of calendering process on NMC622 cathodes using a 3-3-2 full factorial design of experiments. The data set consists of 18 unique combinations of calender roll temperature (85 °C, 120 °C, or 145 °C), electrode porosity (30%, 35%, or 40%), and electrode mass loading (120 g/m² or 180 g/m²). The reported physical characteristics of the electrodes include thickness, coating weight, maximum tensile strength, and density. The electrochemical performances of the electrodes were obtained by testing coin cells. In this context, 54 half-cells were produced, 3 per each calendering experiment to ensure repeatability and reliability of the results. The responses of interest included, charge energy capacity at C/2, C/5, discharge energy capacity at C/20, C/5, C/2, C, 2C, 5C, 10C, gravimetric capacity (charge at C/2, C/5, discharge at C/20, C/5, C/2, C, 2C, 5C, 10C), volumetric capacity (charge at C/2, C/5, discharge at C/20, C/5, C/2, C, 2C, 5C, 10C), rate performance (5C:0.2C), area specific impedance (at 10% to 90% state of charge (SoC) in 10 breakpoints), long-term cycling capacity (charge at C/5 for 50 cycles, discharge at C/2 for 50 cycles), long-term cycling degradation (at C/2 during 50 cycles of charge and discharge), and cycling columbic efficiency (50 cycles of C/2 charge and discharge). The details of the experimental design that has led to this data as well as comprehensive statistical analysis, and machine learning-based models can be found in the recently published manuscripts by Hidalgo et al. and Faraji-Niri et al. [1,2].

Cross-sectional analysis of lithium ion electrodes using spatial autocorrelation techniques.

Join counting, a standard technique in spatial autocorrelation analysis, has been used to quantify the clustering of carbon, fluorine and sodium in cross-sectioned anode and cathode samples. The sample preparation and EDS mapping steps are sufficiently fast for every coating from two Design of Experiment (DoE) test matrices to be characterised. The results show two types of heterogeneity in material distribution; gradients across the coating from the current collector to the surface, and clustering. In the cathode samples, the carbon is more clustered than the fluorine, implying that the conductive carbon component is less well distributed than the binder. The results are correlated with input parameters systematically varied in the DoE e.g. coating blade gap, coating speed, and other output parameters e.g. coat weight, and electrochemical resistance.

Experimental data of cathodes manufactured in a convective dryer at the pilot-plant scale, and charge and discharge capacities of half-coin lithium-ion cells.

Megtec Systems pilot-plant scale continuous convective coater. The data was generated as part of an experimental design involving the following coating-drying process variables and ranges: comma bar gap, 80-140 µm; web speed, 0.5-1.5 m/min; coating ratio, 110-150%; drying temperature, 85-110 °C and drying air speed, 5-15 m/s. The manufacturing data include pre-calendered coating thickness, mass loading dry and wet, pre-calendered porosity, spatial autocorrelation and join counting (SAJC) Z-score for carbon and for fluorine, cell thickness, coating weight and porosity of 15 different electrode coatings and 45 half-coin cells. The electrochemical data was obtained at 25 °C in a Maccor 4000 series battery cycler and consists of charge and discharge capacities at C/20, C/5, C/2, 1C, 2C, 5C and 10C C-rates. Discharge gravimetric and volumetric capacities, rate performance (at 5C:0.2C) and first cycle loss data is also reported. Details of the experimental design and a comprehensive analysis of the data can be found in the co-submitted manuscript (Román-Ramírez et al., 2021). Additional collected data not used in Román-Ramírez et al. (2021) is reported in the present manuscript and include visual observations of coating defects, rheological properties of the electrode slurries (solid content, viscosity, coating shear rate and viscosity at coating shear rate), room temperature and room humidity during the coatings and first cycle loss of the coin cells. Raw and analyzed data is made available. The reported data can be used to extend the analysis reported in Román-Ramírez et al. (2021), and for the comparison of relevant data obtained at different manufacturing scales.

Polarization Screening Mechanisms at La0.7Sr0.3MnO3-PbTiO3 Interfaces.

The structural, electronic, and magnetic properties of interfaces between epitaxial La0.7Sr0.3MnO3 and PbTiO3 have been explored via atomic resolution transmission electron microscopy of a functional multiferroic tunnel junction. Measurements of the polar displacements and octahedral tilting show the competition between the two distortions at the interface and demonstrate strong dependence on the polarization orientation. The density functional theory provides information on the electronic and magnetic properties, where the interface termination plays a crucial role in the screening mechanisms.

Polarization curling and flux closures in multiferroic tunnel junctions.

Formation of domain walls in ferroelectrics is not energetically favourable in low-dimensional systems. Instead, vortex-type structures are formed that are driven by depolarization fields occurring in such systems. Consequently, polarization vortices have only been experimentally found in systems in which these fields are deliberately maximized, that is, in films between insulating layers. As such configurations are devoid of screening charges provided by metal electrodes, commonly used in electronic devices, it is wise to investigate if curling polarization structures are innate to ferroelectricity or induced by the absence of electrodes. Here we show that in unpoled Co/PbTiO3/(La,Sr)MnO3 ferroelectric tunnel junctions, the polarization in active PbTiO3 layers 9 unit cells thick forms Kittel-like domains, while at 6 unit cells there is a complex flux-closure curling behaviour resembling an incommensurate phase. Reducing the thickness to 3 unit cells, there is an almost complete loss of switchable polarization associated with an internal gradient.

In-plane tunnelling field-effect transistor integrated on Silicon.

Silicon has persevered as the primary substrate of microelectronics during last decades. During last years, it has been gradually embracing the integration of ferroelectricity and ferromagnetism. The successful incorporation of these two functionalities to silicon has delivered the desired non-volatility via charge-effects and giant magneto-resistance. On the other hand, there has been a numerous demonstrations of the so-called magnetoelectric effect (coupling between ferroelectric and ferromagnetic order) using nearly-perfect heterostructures. However, the scrutiny of the ingredients that lead to magnetoelectric coupling, namely magnetic moment and a conducting channel, does not necessarily require structural perfection. In this work, we circumvent the stringent requirements for epilayers while preserving the magnetoelectric functionality in a silicon-integrated device. Additionally, we have identified an in-plane tunnelling mechanism which responds to a vertical electric field. This genuine electroresistance effect is distinct from known resistive-switching or tunnel electro resistance.

Four-state ferroelectric spin-valve.

Spin-valves had empowered the giant magnetoresistance (GMR) devices to have memory. The insertion of thin antiferromagnetic (AFM) films allowed two stable magnetic field-induced switchable resistance states persisting in remanence. In this letter, we show that, without the deliberate introduction of such an AFM layer, this functionality is transferred to multiferroic tunnel junctions (MFTJ) allowing us to create a four-state resistive memory device. We observed that the ferroelectric/ferromagnetic interface plays a crucial role in the stabilization of the exchange bias, which ultimately leads to four robust electro tunnel electro resistance (TER) and tunnel magneto resistance (TMR) states in the junction.