New Class of High-Energy, High-Power Capacitive Devices Enabled by Stabilized Lithium Metal Anodes

Lithium-ion capacitors (LIC) combine the energy storage mechanisms of lithium-ion batteries and electric double layer capacitors (EDLC) and are supposed to promise the best of both worlds: high energy and power density combined with a long life. However, the lack of lithium cation sources in the carbon cathode demands the cumbersome step of prelithiation of the graphite anode, mainly by using sacrificial lithium metal, hindering the mass adoption of LICs. Here, in a conceptually new class of devices termed lithium metal capacitors (LMC), we replace the graphite anode with a lithium metal anode stabilized by a complex yet stable solid-electrolyte interface (SEI). Via a specialized formation process, the well-explored synergetic reaction between the LiNO₃ additive and controlled amounts of polysulfides in an ether-based electrolyte stabilizes the SEI on the lithium metal electrode. Optimized devices at the coin cell level deliver 55 mAh g^-1 at a fast 30C discharge rate and maintain 95% capacity after 8000 cycles. At the pouch-cell level, energy densities of 13 Wh kg^-1 are readily achieved, indicating the transferability of the technology to practical scales. The LMC, a new class of capacitive device, eliminates the prelithiation process of the conventional LIC, allowing practical production at scale and offering exciting avenues for exploring versatile cathode chemistries on account of using a lithium metal anode.