Indiana University-Purdue University Indianapolis (IUPUI) / Heat generation is a major safety concern in the design and development of Li ion batteries (LIBs) for large scale applications, such as electric vehicles. The total heat generation in LIBs includes entropic heat, enthalpy, reaction heat, and heat of mixing. The main objective of this study is to investigate the influence of heat of mixing on the LIBs and to understand whether it is necessary to consider the heat of mixing during the design and development of LIBs. In the previous research, Thomas and Newman derived methods to compute heat of mixing in LIB cells. Their results show that the heat of mixing cannot be neglected in comparison with the other heat sources at 2 C rate. In this study, the heat of mixing in different materials, porosity, particle sizes, and charging/discharging rate was investigated. A COMSOL mathematical model was built to simulate the heat generation of LIBs. The LIB model was based on Newman’s model. LiMn2O4 and LiCoO2 were applied as the cathode materials, and LiC6 was applied as the anode material. The results of heat of mixing were compared with the other heat sources to investigate the weight of heat of mixing in the total heat generation. The heat of mixing in cathode is smaller than the heat of mixing in anode, because of the diffusivity of LiCoO2 is 1 ×10-13 m2/s, which is larger than LiC6's diffusivity 2.52 × 10-14 m2/s. In the comparison, the heat of mixing is not as much as the irreversible heat and reversible heat, but it still cannot be neglected. Finally, a special situation will be discussed, which is the heat of mixing under the relaxation status. For instance, after the drivers turn off their vehicles, the entropy, ix enthalpy and reaction heat in LIBs will stop generating, but the heat will still be generated due to the release of heat of mixing. Therefore, it is meaningful to investigate to see if this process has significant influence on the safety and cycle life of LIBs.

Indiana University-Purdue University Indianapolis (IUPUI) / Lithium-ion batteries are widely used for portable electronics due to high energy density, mature processing technology and reduced cost. However, their applications are somewhat limited by safety concerns. The lithium-ion battery users will take risks in burn or explosion which results from some internal components failure. So, a practical method is required urgently to find out the failures in early time. In this thesis, a new method based on temperature difference between internal point and surface (TDIS) of the battery is developed to detect the thermal failure especially the thermal runaway in early time. A lumped simple thermal model of a lithium-ion battery is developed based on TDIS. Heat transfer coefficients and heat capacity are determined from simultaneous measurements of the surface temperature and the internal temperature in cyclic constant current charging/discharging test. A look-up table of heating power in lithium ion battery is developed based on the lumped model and cyclic charging/discharging experimental results in normal operating condition. A failure detector is also built based on TDIS and reference heating power curve from the look-up table to detect aberrant heating power and bad parameters in transfer function of the lumped model. The TDIS method and TDIS detector is validated to be effective in thermal runaway detection in a thermal runway experiment. In the validation of thermal runway test, the system can find the abnormal heat generation before thermal runaway happens by detecting both abnormal heating power generation and parameter change in transfer function of thermal model of lithium ion batteries. The result of validation is compatible with the expectation of detector design. A simple and applicable detector is developed for lithium ion battery catastrophic failure detection.