Doctor of Philosophy (PhD)
Materials Science and Engineering
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Sulfur, Polysulfides, Nitrogen-doped graphene, Manganese sulfide, Lithium-sulfur batteries, Room-temperature sodium-sulfur batteries, Cathode, Anode, Nanocomposites
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Developing next generation secondary batteries has attracted much attention in recent years due to the increasing demand of high energy and high power density energy storage for portable electronics, electric vehicles and renewable sources of energy. This dissertation investigates sulfur based advanced electrode materials in Lithium/Sodium batteries. The electrochemical performances of the electrode materials have been enhanced due to their unique nano structures as well as the formation of novel composites.
First, a nitrogen-doped graphene nanosheets/sulfur (NGNSs/S) composite was synthesized via a facile chemical reaction deposition. In this composite, NGNSs were employed as a conductive host to entrap S/polysulfides in the cathode part. The NGNSs/S composite delivered an initial discharge capacity of 856.7 mAh g-1 and a reversible capacity of 319.3 mAh g-1 at 0.1C with good recoverable rate capability.
Second, NGNS/S nanocomposites, synthesized using chemical reaction-deposition method and low temperature heat treatment, were further studied as active cathode materials for room temperature Na-S batteries. Both high loading composite with 86% gamma-S8 and low loading composite with 25% gamma-S8 have been electrochemically evaluated and compared with both NGNS and S control electrodes. It was found that low loading NGNS/S composite exhibited better electrochemical performance with specific capacity of 110 and 48 mAh g-1 at 0.1C at the 1st and 300th cycle, respectively. The Coulombic efficiency of 100% was obtained at the 300th cycle.
Third, high purity rock-salt (RS), zinc-blende (ZB) and wurtzite (WZ) MnS nanocrystals with different morphologies were successfully synthesized via a facile solvothermal method. RS-, ZB- and WZ-MnS electrodes showed the capacities of 232.5 mAh g-1, 287.9 mAh g-1 and 79.8 mAh g-1 at the 600th cycle, respectively. ZB-MnS displayed the best performance in terms of specific capacity and cyclability. Interestingly, MnS electrodes exhibited an unusual phenomenon of capacity increase upon cycling which was ascribed to the decreased cell resistance and enhanced interfacial charge storage.
In summary, this dissertation provides investigation of sulfur based electrode materials with sulfur/N-doped graphene composites and MnS nanocrystals. Their electrochemical performances have been evaluated and discussed. The understanding of their reaction mechanisms and electrochemical enhancement could make progress on development of secondary batteries.
Hao, Yong, "Sulfur Based Electrode Materials For Secondary Batteries" (2016). FIU Electronic Theses and Dissertations. 2582.
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