PMID- 38336365 OWN - NLM STAT- Publisher LR - 20240220 IS - 1521-4095 (Electronic) IS - 0935-9648 (Linking) DP - 2024 Feb 9 TI - Anion-Reinforced Solvating Ionic Liquid Electrolytes Enabling Stable High-Nickel Cathode in Lithium-Metal Batteries. PG - e2400537 LID - 10.1002/adma.202400537 [doi] AB - Ionic liquid electrolytes (ILEs) are promising to develop high-safety and high-energy-density lithium-metal batteries (LMBs). Unfortunately, ILEs normally face the challenge of sluggish Li(+) transport due to increased ions' clustering caused by Coulombic interactions. Here a type of anion-reinforced solvating ILEs (ASILEs) is discovered, which reduce ions' clustering by enhancing the anion-cation coordination and promoting more anions to enter the internal solvation sheath of Li(+) to address this concern. The designed ASILEs, incorporating chlorinated hydrocarbons and two anions, bis(fluorosulfonyl) imide (FSI(-) ) and bis(trifluoromethanesulfonyl) imide (TFSI(-) ), aim to enhance Li(+) transport ability, stabilize the interface of the high-nickel cathode material (LiNi(0.8) Co(0.1) Mn(0.1) O(2) , NCM811), and retain fire-retardant properties. With these ASILEs, the Li/NCM811 cell exhibits high initial specific capacity (203 mAh g(-1) at 0.1 C), outstanding capacity retention (81.6% over 500 cycles at 1.0 C), and excellent average Coulombic efficiency (99.9% over 500 cycles at 1.0 C). Furthermore, an Ah-level Li/NCM811 pouch cell achieves a notable energy density of 386 Wh kg(-1) , indicating the practical feasibility of this electrolyte. This research offers a practical solution and fundamental guidance for the rational design of advanced ILEs, enabling the development of high-safety and high-energy-density LMBs. CI - (c) 2024 Wiley-VCH GmbH. FAU - Zou, Wenhong AU - Zou W AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. FAU - Zhang, Jun AU - Zhang J AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. FAU - Liu, Mengying AU - Liu M AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. FAU - Li, Jidao AU - Li J AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. FAU - Ren, Zejia AU - Ren Z AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. FAU - Zhao, Wenlong AU - Zhao W AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. AD - CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Science, Suzhou, 215123, China. FAU - Zhang, Yanyan AU - Zhang Y AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. FAU - Shen, Yanbin AU - Shen Y AD - CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Science, Suzhou, 215123, China. FAU - Tang, Yuxin AU - Tang Y AUID- ORCID: 0000-0001-9348-323X AD - College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, China. AD - Qingyuan Innovation Laboratory, Quanzhou, 362801, China. LA - eng GR - 2022YFE0206400/National Key Research and Development Program of China/ GR - 22279017/National Natural Science Foundation of China/ GR - 00623001/Platform Supporting Fund of Qingyuan Innovation Laboratory/ GR - 00223002/Key Program of Qingyuan Innovation Laboratory/ PT - Journal Article DEP - 20240209 PL - Germany TA - Adv Mater JT - Advanced materials (Deerfield Beach, Fla.) JID - 9885358 SB - IM OTO - NOTNLM OT - anion reinforced OT - high energy density OT - ionic liquids OT - lithium-metal batteries EDAT- 2024/02/10 13:18 MHDA- 2024/02/10 13:18 CRDT- 2024/02/09 20:33 PHST- 2024/02/05 00:00 [revised] PHST- 2024/01/11 00:00 [received] PHST- 2024/02/10 13:18 [pubmed] PHST- 2024/02/10 13:18 [medline] PHST- 2024/02/09 20:33 [entrez] AID - 10.1002/adma.202400537 [doi] PST - aheadofprint SO - Adv Mater. 2024 Feb 9:e2400537. doi: 10.1002/adma.202400537.