|Authors:||Dries De Sloovere, Danny E. P. Vanpoucke, Andreas Paulus, Bjorn Joos, Lavinia Calvi, Thomas Vranken, Gunter Reekmans, Peter Adriaensens, Nicolas Eshraghi, Abdelfattah Mahmoud, Frédéric Boschini, Mohammadhosein Safari, Marlies K. Van Bael, An Hardy|
|Journal:||Advanced Energy and Sustainability Research 3(3), 2100159 (2022)|
|Graphical Abstract: Understanding the electronic structure of Na-TFSI interacting with NMA.|
Sodium-ion batteries are alternatives for lithium-ion batteries in applications where cost-effectiveness is of primary concern, such as stationary energy storage. The stability of sodium-ion batteries is limited by the current generation of electrolytes, particularly at higher temperatures. Therefore, the search for an electrolyte which is stable at these temperatures is of utmost importance. Here, we introduce such an electrolyte using non-flammable deep eutectic solvents, consisting of sodium bis(trifluoromethane)sulfonimide (NaTFSI) dissolved in N-methyl acetamide (NMA). Increasing the NaTFSI concentration replaces NMA-NMA hydrogen bonds with strong ionic interactions between NMA, Na+, and TFSI–. These interactions lower NMA’s HOMO energy level compared to that of TFSI–, leading to an increased anodic stability (up to ~4.65 V vs Na+/Na). (Na3V2(PO4)2F3/CNT)/(Na2+xTi4O9/C) full cells show 74.8% capacity retention after 1000 cycles at 1 C and 55 °C, and 97.0% capacity retention after 250 cycles at 0.2 C and 55 °C. This is considerably higher than for (Na3V2(PO4)2F3/CNT)/(Na2+xTi4O9/C) full cells containing a conventional electrolyte. According to the electrochemical impedance analysis, the improved electrochemical stability is linked to the formation of more robust surface films at the electrode/electrolyte interface. The improved durability and safety highlight that deep eutectic solvents can be viable electrolyte alternatives for sodium-ion batteries.