Beyond Li ion: Rechargeable Metal Batteries based on Multivalent Chemistry

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Gao, Tao
Wang, Chunsheng
The development of advanced battery technology with lower cost and higher energy density is important since various mobile applications are becoming indispensable in our daily life. While Li chemistry has approached its theoretical limit after several decades’ increment improvement, the potential of multivalent chemistry (Mg, Al, etc.) remains unexplored. Compared to Li ion chemistry, multivalent chemistry provides many intriguing benefits in terms of lowering cost and increasing energy density. First of all, minerals containing multivalent element such as Mg, Al, and etc. are much more abundant and cheaper than Li. Second, multivalent metals (Mg, Al etc.) can be directly used as anode materials, ensuring much higher anode capacity than graphite currently used in Li-ion battery. Third, the divalent or trivalent nature of the electroactive cation (Mg2+and Al3+) also promise high capacity for intercalation cathodes because the capacity of these materials are limited by their available ion occupancy sites in the crystal structure instead of its capability to accept electrons. In this dissertation, I detailed our efforts in examining some redox chemistries and materials for the use of rechargeable batteries based on multivalent metal anodes. They include intercalation cathode (TiS2) and conversion cathode (sulfur, iodine). We studied their electrochemical redox behavior in the corresponding chemistry, the thermodynamics, kinetics as well as the reaction reversibility. The reaction mechanism is also investigated with various macroscopic and spectroscopic techniques.