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State-of-health estimates of batteries are essential for onboard electric vehicles in order to provide safe, reliable, and cost-effective battery operation. This paper suggests a method to estimate the 10-s discharge resistance, which is an established battery figure of merit from laboratory testing, without performing the laboratory test. Instead, a state-of-health estimate of batteries is obtained using data directly from their operational use, e.g., onboard electric vehicles. It is shown that simple dynamical battery models, based on a current input and a voltage output, with model parameters dependent on temperature and state of charge, can be derived using AutoRegressive with eXogenous input models, whose order can be adjusted to describe the complex battery behavior. Then, the 10-s discharge resistance can be conveniently computed from the identified model parameters. Moreover, the uncertainty of the estimated resistance values is provided by the method. The suggested method is validated with usage data from emulated electric vehicle operation of an automotive lithium-ion battery cell. The resistance values are estimated accurately for a state-of-charge and temperature range spanning typical electric vehicle operating conditions. The identification of the model parameters and the resistance computation are very fast, rendering the method suitable for onboard application., QC 20180531

Beyond conductivity and viscosity, little is often known about the mass transport properties of next generation lithium battery electrolytes, thus, making performance estimation uncertain when concentration gradients are present, as conductivity only describes performance in the absence of these gradients. This study experimentally measured the diffusion resistivity, originating from voltage loss due to a concentration gradient, together with the ohmic resistivity, obtained from ionic conductivity measurements, hence, evaluating electrolytes both with and without the presence of concentration gradients. Under galvanostatic conditions, the concentration gradients, of all electrolytes examined, developed quickly and the diffusion resistivity rapidly dominated the ohmic resistivity. The electrolytes investigated consisted of lithium salt in: room temperature ionic liquids (RTIL), RTIL mixed organic carbonates, dimethyl sulfoxide (DMSO), and a conventional Li-ion battery electrolyte. At steady state the RTIL electrolytes displayed a diffusion resistivity similar to 20 times greater than the ohmic resistivity. The DMSO-based electrolyte showed mass transport properties similar to the conventional Li-ion battery electrolyte. In conclusion, the results presented in this study show that the diffusion polarization must be considered in applications where high energy and power density are desired., QC 20180116

The industrial lignin used here is a byproduct from Kraft pulp mills, extracted from black liquor. Since lignin is inexpensive, abundant and renewable, its utilization has attracted more and more attention. In this work, lignin was used for the first time as binder material for LiFePO4 positive and graphite negative electrodes in Li-ion batteries. A procedure for pretreatment of lignin, where low-molecular fractions were removed by leaching, was necessary to obtain good battery performance. The lignin was analyzed for molecular mass distribution and thermal behavior prior to and after the pretreatment. Electrodes containing active material, conductive particles and lignin were cast on metal foils, acting as current collectors and characterized using scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS) and galvanostatic charge-discharge cycles. Good reversible capacities were obtained, 148 mAh·g-1 for the positive electrode and 305 mAh·g-1 for the negative electrode. Fairly good rate capabilities were found for both the positive electrode with 117 mAh·g-1 and the negative electrode with 160 mAh·g-1 at 1C. Low ohmic resistance also indicated good binder functionality. The results show that lignin is a promising candidate as binder material for electrodes in eco-friendly Li-ion batteries.

Thermal effects are linked to all main barriers to the widespread commercialization of lithium-ion battery powered vehicles. This paper presents a coupled 2D electrochemical - 3D thermal model of a large-format prismatic lithium-ion battery, including a thermal management system with a heat sink connected to the surface opposite the terminals, undergoing the dynamic current behavior of a plug-in hybrid electric (PHEV) vehicle using a load cycle with a maximum current of 8 C, validated using potential and temperature data. The model fits the data well, with small deviations at the most demanding parts of the cycle. The maximum temperature increase and temperature difference of the jellyroll is found to be 9.7 degrees C and 3.6 degrees C, respectively. The electrolyte is found to limit the performance during the high-current pulses, as the concentration reaches extreme values, leading to a very uneven current distribution. Two other thermal management strategies, short side and long side surfaces cooling, are evaluated but are found to have only minor effects on the temperature of the jellyroll, with maximum jellyroll temperatures increases of 9.4 degrees C and 8.1 degrees C, respectively, and maximum temperature differences of 3.7 degrees C and 5.0 degrees C, respectively., Updated from Manuscript to Article. QC 20160202

Flexible Li-ion batteries attract increasing interest for applications in bendable and wearable electronic devices. TEMPO-oxidized cellulose nanofibrils (TOCNF), a renewable material, is a promising candidate as binder for flexible Li-ion batteries with good mechanical properties. Paper batteries can be produced using a water-based paper making process, avoiding the use of toxic solvents. In this work, finely dispersed TOCNF was used and showed good binding properties at concentrations as low as 4 wt %. The TOCNF was characterized using atomic force microscopy and found to be well dispersed with fibrils of average widths of about 2.7 nm and lengths of approximately 0.1-1 mu m. Traces of moisture, trapped in the hygroscopic cellulose, is a concern when the material is used in Li-ion batteries. The low amount of binder reduces possible moisture and also increases the capacity of the electrodes, based on total weight. Effects of moisture on electrochemical battery performance were studied on electrodes dried at 110 degrees C in a vacuum for varying periods. It was found that increased drying time slightly increased the specific capacities of the LiFePO4 electrodes, whereas the capacities of the graphite electrodes decreased. The Coulombic efficiencies of the electrodes were not much affected by the varying drying times. Drying the electrodes for 1 h was enough to achieve good electrochemical performance. Addition of vinylene carbonate to the electrolyte had a positive effect on cycling for both graphite and LiFePO4. A failure mechanism observed at high TOCNF concentrations is the formation of compact films in the electrodes., QC 20161129

The performance difference between commercial and laboratory scale cells remains a problem to be solved. Different way of battery electrode preparation is considered to be the main reason underlying various battery performance. In this work, the effect of slurry composition on electrochemical properties of Li-ion batteries is reported. Slurry preparation with various compositions of LiFePO4 active material (76-88%), PVdF binder (6-12%) and Super P Carbon conductive additive (6-12%) has been studied. Charge-discharge curves and capacity fade of electrodes are also investigated. Selected electrodes were pressed in order to see the effect of pressing on the final performance. Results showed that varying PVdF and carbon content mainly effects charge-discharge characteristics. For unpressed samples, higher amount of PVdF and carbon could result higher maximum specific capacity and lower internal resistance during lithiation and delithiation of positive electrode. Pressing reduces the distance between slurry particles, which enhances the conductivity of the prepared cell., QC 20151116

This paper describes an experimental setup for investigating the effects of current ripple on lithium-ion battery cells. The experimental setup is designed so that twelve li-ion cells can be simultaneously tested in a controlled environment. The experimental setup allows for a wide range of current ripple in terms of frequency and amplitude. Additionally, the quantification of the current ripple effects such as the aging of li-ion cells implies that a precise measurement system has to be designed which also are discussed in the paper., QC 20160216

This paper presents results from a field test performed on commercial power-optimized lithium-ion battery cells cycled on three heavy-duty trucks. The goal with this study was to age battery cells in a hybrid electric vehicle (HEV) environment and find suitable methods for identifying cell ageing. The battery cells were cycled on in-house developed equipment intended for testing on conventional vehicles by emulating an HEV environment. A hybrid strategy that allows battery usage to vary within certain limits depending on driving patterns was used. This concept allows unobtrusive and low-cost testing of battery cells under realistic conditions. Each truck was equipped with one cell cycling equipment and two battery cells. One cell per vehicle was cycled during the test period while a reference cell on each vehicle experienced the same environmental conditions without being cycled. Differential voltage analysis and electrochemical impedance spectroscopy were used to identify ageing of the tested battery cells. Analysis of driving patterns and battery usage was performed from collected vehicle data and battery cell data., QC 20150825. Updated from Manuscript to Article in journal.

Superconcentration of aprotic electrolytes has recently emerged as a way to stabilize solvents that otherwise would be impossible to use, in e.g. lithium-ion batteries (LIBs). As demanding applications, such as hybrid electric vehicles and fast charging, become increasingly important, battery manufacturers are struggling to find a suitable electrolyte able to deliver high power with low polarization. Electrolyte characterizations able to accurately predict the high-power performance of such electrolytes are also of utmost importance. This study reports a full.characterization of the mass-transport phenomena for a superconcentrated LiTFSL-acetonitrile electrolyte in concentrations ranging from 2.7 M to 4.2 M. The method obtains the ionic conductivity, cationic transport number, diffusion coefficient, and the thermodynamic enhancement factor, by combining mathematical modeling and three electrochemical experiments. Furthermore, the density and the viscosity were measured. The transport number with respect to the room is found to be very high compared to other liquid LIB electrolytes, but a low diffusion coefficient lowers overall performance. The ionic conductivity decreases quickly with concentration, dropping from 12.7 mS/cm at 2.7 M to 0.76 mS/cm at 4.2 M. Considering all the effects in terms of the mass-transport of the electrolyte, the lower end of the studied concentration range is favorable., QC 20150522

Mass transport in the electrolyte is one of the limiting processes when it comes to the power density and energy efficiency of lithium-ion batteries. Electrolyte characterizations are therefore of utmost importance. This study reports the ionic conductivity, diffusion coefficient, lithium-ion transport number, and thermodynamic enhancement factor, as well as density and viscosity, for the electrolyte LiPF6 in EC:DEC (1 1, by weight) at 10 degrees C, 25 degrees C, and 40 degrees C and for concentrations between 0.5 M and 1.5 M. By combining mathematical modeling and three experiments: conductivity measurements, concentration cells, and galvanostatic polarizations, the mass transport phenomena were fully characterized. All parameters were found to vary strongly with both concentration and temperature proving that temperature dependent parameters are essential when studying thermal behavior of lithium-ion batteries. Moreover, conductivity increased with temperature and showed a local maximum at around 1 M within the concentration range at all temperatures. The other parameters either showed a continuous decrease (diffusion coefficient and lithiumion transport number) or increase (thermodynamic enhancement factor) with concentration at all temperatures. Limited liquid range leading to solvent crystallization at 10 degrees C leads to very poor performance, possibly due to the strong coordination between the lithium ion and the crystallizing species, EC. Overall, the studied electrolyte is found to perform poorly compared to previously studied systems., QC 20150331

In this study, metal nitrides MN (M = Cr, Co) nanoparticles of particle size similar to 20-30 nm have been prepared under NH3 + N-2 atmosphere at relatively low temperature. The Cr-urea complex was directly converted to CrN with an intermediate formation of Cr2O3, whereas CoN was prepared from Co3O4. These compounds were characterized by X-ray diffraction (XRD) and high resolution transmission electron microscopy (HR-TEM) techniques. The electrochemical properties were evaluated by galvanostatic cycling, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The electrochemical performance of the resultant MN nanoparticles showed that they can be used as potential electrode materials for non-aqueous hybrid electrochemical supercapacitors (HESCs). The MN/AC showed high specific capacitance of 75 and 37 F g (1) for M = Cr, Co, respectively when cycled at 30 mA g (1) in non-aqueous electrolyte., QC 20150713

During long and high current pulses, diffusion resistance becomes important in lithium-ion batteries. In such diffusion-intense situations, a static support vector machine-based battery model relying on instantaneous current, state-of-charge (SOC), and temperature is not sufficient to capture the time-dependent voltage characteristics. In order to account for the diffusion-related voltage dynamics, we suggest therefore the inclusion of current history in the data-driven battery model by moving averages of the recent current. The voltage estimation performance of six different dynamic battery models with additional current history input is studied during relevant test scenarios. All current history models improve the time-dependent voltage drop estimation compared to the static model, manifesting the beneficial effect of the additional current history input during diffusion-intense situations. The best diffusion resistance estimation results are obtained for the two-step voltage estimation models that incorporate a reciprocal square root of time weighing function for the current of the previous 100 s or an exponential time function with a 20 s time constant (1–8% relative error). Those current history models even improve the overall voltage estimation performance during the studied test scenarios (under 0.25% root-mean-square percentage error)., QC 20150914

We have built an experimental setup which exposes twelve cells to a well-defined ripple current. It consists of a system for cycling high capacity cells in parallel with a triangular current waveform superimposed on top of the direct current. The frequency of the waveform is variable up to 50 Hz, and the sum of the DC and AC components can have a magnitude of -40 A to 40 A. Current is measured over a 500 μω shunt resistor. The voltage and current of each cell is read simultaneously at a sample rate up to 4 MS/s, allowing for precise impedance measurements even for high frequency harmonics. The cells are cycled at 40 °C. The experiment has been designed to eliminate indirect effects of the AC harmonics as far as possible. This system is being used to test whether or not AC harmonics affect Li-ion aging., QC 20160523

This study presents an extensive characterization of a standard Li-ion battery (LiB) electrolyte containing different concentrations of the flame retardant triphenyl phosphate (TPP) in the context of high power applications. Electrolyte characterization shows only a minor decrease in the electrolyte flammability for low TPP concentrations. The addition of TPP to the electrolyte leads to increased viscosity and decreased conductivity. The solvation of the lithium ion charge carriers seem to be directly affected by the TPP addition as evidenced by Raman spectroscopy and increased mass-transport resistivity. Graphite/LiFePO4 full cell tests show the energy efficiency to decrease with the addition of TPP. Specifically, diffusion resistivity is observed to be the main source of increased losses. Furthermore, TPP influences the interface chemistry on both the positive and the negative electrode. Higher concentrations of TPP lead to thicker interface layers on LiFePO4. Even though TPP is not electrochemically reduced on graphite, it does participate in SEI formation. TPP cannot be considered a suitable flame retardant for high power applications as there is only a minor impact of TPP on the flammability of the electrolyte for low concentrations of TPP, and a significant increase in polarization is observed for higher concentrations of TPP.

Capacity and resistance are state-of-health (SOH) indicators that are essential to monitor during the application of batteries on board electric vehicles. For state-of-health determination in laboratory environment, standard battery performance tests are established and well-functioning. Since standard performance tests are not available on-board a vehicle, we are developing a method where those standard tests are applied virtually to a support vector machine-based battery model. This data-driven model is solely based on variables available during ordinary electric vehicle (EV) operation such as battery current, voltage and temperature. This article contributes with a thorough experimental validation of this method, as well as the introduction of new features capacity estimation and temperature dependence. Typical EV battery usage data is generated and exposed to the suggested method in order to estimate capacity and resistance. These estimations are compared to direct measurements of the SOH indicators with standard tests. The obtained estimations of capacities and instantaneous resistances demonstrate good accuracy over a temperature and state-of-charge range typical for EV operating conditions and allow thus for online detection of battery degradation. The proposed method is also found to be suitable for on-board application in respect of processing power and memory restrictions., QC 20141118

Commercial battery cells with Li4Ti5O12 negative electrode and composite metal oxide positive electrode have been analyzed with respect to aging mechanisms. Electrochemical impedance spectroscopy (EIS), differential capacity analysis (dQ/dV), differential voltage analysis (dV/dQ) and scanning electron microscopy (SEM) with energy dispersive X-ray analysis (EDX) were used to identify different ageing mechanisms such as lithium inventory loss, loss of active electrode material and surface film growth. The active material of the positive electrode was also examined by X-ray diffraction (XRD). Aging mechanisms were studied for both calendar-aged and cycle-aged cells. Data from half cells prepared from post mortem harvested electrode material, using lithium foil as negative electrode and pouch material as encapsulation, were used as reference to full cell data. Electrochemical analysis of full and half cells combined with material analysis showed to be a powerful method to identify aging mechanisms in this type of commercial cells. The calendar-aged cell showed insignificant aging while the cycle-aged cell showed noticeable loss of positive electrode active material and loss of cyclable lithium, but only minor loss of negative electrode active material. The results imply that Li4Ti5O12 negative electrode material is a good alternative to other materials if high energy density is not the primary goal., QC 20141106

This study was based on developing Li(Ni1/3Mn1/3Co(1/3-x)Mx)O-2, (M = Mg, Fe, Al and x = 0 to 0.33) materials by substituting expensive Co content in this NMC system with cheaper Mg, Fe and Al additives for the cathode application in rechargeable lithium ion batteries (LIB). The Pechini method, which is a low-cost wet chemical technique, was used for powder synthesis in this study. The XRD phase analysis revealed the formation of solid solutions of appropriate layered Li(Ni1/3Mn1/3Co(1/3-x)Mx)O-2 phase.of R-3m structure in the prepared compositions over x = 0.11 substitution of Fe and Mg. Furthermore, these Fe and Mg substituted compositions showed considerably higher electrical conductivity than the base material Li(Ni1/3Mn1/3Co(1/3-x)Mx)O-2 (over 0.9 x 10(-5) S/cm at 25 degrees C). In the cell studies, the Fe and Mg substituted compositions with x = 0.11 showed a specific capacity of 122 and 125 mAhg(-1), respectively, which are comparable to the specific capacity of the state-of-the-art LiCoO2 cathode material of LIB. Altogether, this study shows the ability of preparing these NMC materials by Pechini method with appropriate structural and electrochemical properties suitable for the LIB cathode., QC 20150209