The anode solid electrolyte interface (SEI) on the anode of lithium ion batteries contains lithium carbonate (Li2CO3), lithium methyl carbonate (LMC), and lithium ethylene dicarbonate (LEDC). The development of a strong physical understanding of the properties of the SEI requires a strong understanding of the evolution of the SEI composition over extended timeframes. The thermal stability of Li2CO3, LMC, and LEDC in the presence of LiPF6 in dimethyl carbonate (DMC), a common salt and solvent, respectively, in lithium ion battery electrolytes, has been investigated to afford a better understanding of the evolution of the SEI. The residual solids from the reaction mixtures have been characterized by a combination of X-ray photoelectron spectroscopy (XPS) and infrared spectroscopy with attenuated total reflectance (IR-ATR), while the solution and evolved gases have been investigated by nuclear magnetic resonance (NMR) spectroscopy and gas chromatography with mass selective detection (GC-MS). The thermal decomposition of Li2CO3 and LiPF6 in DMC yields CO2, LiF, and F2PO2Li. The thermal decomposition of LMC and LEDC with LiPF6 in DMC results in the generation of a complicated mixture including CO2, LiF, ethers, phosphates, and fluorophosphates.

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This paper covers details of systematic investigation of the thermodynamics (entropy and enthalpy) of intercalation associated with lithium ion in a structurally novel carbon, called Randomly Oriented High Graphene (ROHG) carbon and graphite. Equilibrated OCV (Open Circuit Voltage) versus temperature relationship is investigated to determine the thermodynamic changes with the lithium intercalation. ROHG carbon shows entropy of 9.36 J⋅mol −1 ⋅K −1 and shows no dependency on the inserted lithium concentration. Graphite shows initial entropy of 84.27 J⋅mol −1 ⋅K −1 and shows a strong dependence on lithium concentration. ROHG carbon (from −90.85 kJ mol −1 to −2.88 kJ mol −1 ) shows gradual change in the slope of enthalpy versus lithium ion concentration plot compared to graphite (−48.98 kJ mol −1 to 1.84 kJ mol −1 ). The study clearly shows that a lower amount of energy is required for the lithium ion intercalation into the ROHG structure compared to graphite structure. Randomly oriented graphene platelet cluster structure of ROHG carbon makes it easier for the intercalation or deintercalation of lithium ion. The ease of intercalation and the small cluster structure of ROHG as opposed to the long linear platelet structure of graphite lead to higher rates of the charge-discharge process for ROHG, when used as an electrode material in electrochemical applications.

The structure of carbon material comprising the anode is the key to the performance of a lithium ion capacitor. In addition to determining the capacity, the structure of the carbon material also determines the diffusion rate of the lithium ion into the anode which in turn controls power density which is vital in high rate applications. This paper covers details of systematic investigation of the performance of a structurally novel carbon, called Randomly Oriented High Graphene (ROHG) carbon, and graphite in a high rate application device, that is, lithium ion capacitor. Electrochemical impedance spectroscopy shows that ROHG is less resistive and has faster lithium ion diffusion rates (393.7 × 10−3 S·s(1/2)) compared to graphite (338.1 × 10−3 S·s(1/2)). The impedance spectroscopy data is supported by the cell data showing that the ROHG carbon based device has energy density of 22.8 Wh/l with a power density of 4349.3 W/l, whereas baseline graphite based device has energy density of 5 Wh/l and power density of 4243.3 W/l. This data clearly shows advantage of the randomly oriented graphene platelet structure of ROHG in lithium ion capacitor performance.

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