Abstract

Developing battery systems that are inexpensive, enduring, and safe is essential for integrating renewable energy sources such as solar and wind power into the electricity grid and providing valuable grid services such as frequency regulation, peak shaving, and arbitrage. In this regard, Na-based batteries are promising candidates because they use naturally abundant sodium (Na) as the charge carrier, which can potentially reduce the materials cost and support multiple energy storage applications. Among various Na-based batteries developed to date, thorough investigations have been done on high-temperature (~300°C) Na-metal halide (Na-MH) batteries, which offer long cycle life and superior safety. In particular, the tubular sodium-nickel chloride (Na-NiCl2 or Zebra) battery has been commercialized and found wide application in the telecom and oil/gas industries. However, the high operating temperature and cost of the Zebra battery has hindered its further market penetration. Considering constraints of the Ni-based cell chemistry, it is highly desirable to develop an alternate cathode for Na-MH batteries towards next-generation energy storage applications. This pursuit, unsurprisingly, led us to the Fe/NaCl cathode. In this study, we present an advanced Na-FeCl2 battery with unprecedented high-rate performance and low cost for stationary energy storage applications. Operated at an extremely high current density of 33.3 mA/cm2 at 190°C, the cell can output 74% of its total capacity—a capacity retention double that of IT Na-NiCl2 cells. The origin of the high rate capability of Na-FeCl2 batteries was elucidated by means of comprehensive phase/structure analysis and electrochemical/electroanalytical characterizations. Moreover, Fe particle pulverization originating from liquid-phase reactions was determined to be the major source of capacity fading during long-term cycling. Accordingly, we designed a unique cathode with Ni additive, which delivered a high discharge specific energy density of over 295 Wh/kg for 200 cycles at C/5 with almost no capacity fading.

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