Natrium super ion conductors (NaSICONs), Na1+xZr2SixP3-xO12 (0 ≤ x ≤ 3) are compounds that commonly used as solid electrolytes and membranes... Show moreNatrium super ion conductors (NaSICONs), Na1+xZr2SixP3-xO12 (0 ≤ x ≤ 3) are compounds that commonly used as solid electrolytes and membranes of sodium based batteries, or in gas sensors and fuel cells due to their high sodium ion conductivity, low thermal expansion, and ability to accommodate ions in the lattice. However, NaSICON with high relative density (> 97%) and minimum impurity phases is found to be very difficult to obtain. Furthermore, the cost of the general synthesis methods is a serious drawback. Multi-high-temperature heating procedures is often employed to increase the density and to attain the single phase NaSICON because the particle size and free ZrO2 are better reduced. This research explores the possibility of densification and synthesis of NaSICON in one high-temperature reaction through a novel process termed Integrated Mechanical and Thermal Activation (IMTA) and the co-sintering behavior as well as the NaSICON composite membranes from tape casting. The sintering temperature of NaSICON was decreased by mechanical activation at room temperature using high-energy ball milling. Sintered NaSICON-based materials showed highest total ionic conductivity of 1.45 × 10-3 S cm-1 at room temperature and high density of 3.155 g cm-3 (96.5%). An alternative to obtaining full densification (99%) of NaSICON ceramics was developed utilizing traditional solid-state reaction. This sintered NaSICON without any sintering aid exhibited the total conductivity, 6.59 × 10-4 S cm-1 at 25 °C, and the highest density of 3.238 g cm-3, a better than 2.6% enhancement from the original samples.The second part of the work has comprised of successful fabrication of NaSICON/polymer composite membranes and bi-layered NaSICON/stainless steel membranes to enhance the mechanical flexibility of pure NaSICON films. The effect of different particle sizes of stainless steel on the sintering behavior and shrinkage rate were studied systematically. The effect of solid content in the slurry was also studied to control the density of both support layer and NaSICON body. The affect structural ratios have on co-sintered tapes along with ionic conductivity was investigated using Electrochemical Impedance Spectroscopy (EIS). The co-sintered membrane exhibited a total conductivity as high as 4.580 × 10-4 S/cm at room temperature. EIS results showed the high Na-ions conductivity strongly depends on the feature of grain boundary and the high densification of NaSICON layer. Show less
