High-energy silicon-sulfurized poly(acrylonitrile) battery based on a nitrogen evolution reaction

The practical application of high-energy lithium-sulfur battery is plagued with two deadly obstacles. One is the "shuttle effect" originated from the sulfur cathode, and the other is the low Coulombic efficiency and security issues arising from the lithium metal anode. In addressing these issues, we propose a novel silicon-sulfurized poly(acrylonitrile) full battery. In this lithium metal-free system, the Li source is pre-loaded in the cathode, using a nitrogen evolution reaction (NER) to implant Li⁺ into the silicon/carbon anode. Sulfurized poly(acrylonitrile) based on a solid-solid conversion mechanism can fundamentally circumvent the "shuttle effect". Meanwhile, the silicon/carbon anode can achieve more efficient utilization and higher security when compared with the Li metal anode. The full cell used in this technology can deliver a capacity of 1169.3 mAh g^-1, and it can be stabilized over 100 cycles, implying its excellent electrochemical stability. Furthermore, the practical pouch cell with a high sulfur loading of 4.2 mg cm^-2 can achieve a high specific energy of 513.2 Wh kg^-1. The mechanism of the NER in cathode has also been investigated and analyzed by in situ methods. Notably, this battery design completely conforms to the current battery production technology because of the degassing of gasbag, resulting in a low manufacturing cost. This work will open the avenue to develop a lithium metal-free battery using the NER.