PMID- 38412508 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20240313 IS - 1520-5126 (Electronic) IS - 0002-7863 (Linking) VI - 146 IP - 10 DP - 2024 Mar 13 TI - Ternary Eutectic Electrolyte-Assisted Formation and Dynamic Breathing Effect of the Solid-Electrolyte Interphase for High-Stability Aqueous Magnesium-Ion Full Batteries. PG - 7018-7028 LID - 10.1021/jacs.4c00227 [doi] AB - Aqueous rechargeable magnesium batteries hold immense potential for intrinsically safe, cost-effective, and sustainable energy storage. However, their viability is constrained by a narrow voltage range and suboptimal compatibility between the electrolyte and electrodes. Herein, we introduce an innovative ternary deep eutectic Mg-ion electrolyte composed of MgCl(2).6H(2)O, acetamide, and urea in a precisely balanced 1:1:7 molar ratio. This formulation was optimized by leveraging competitive solvation effects between Mg(2+) ions and two organic components. The full batteries based on this ternary eutectic electrolyte, Mn-doped sodium vanadate (Mn-NVO) anode, and copper hexacyanoferrate cathode exhibited an elevated voltage plateau and high rate capability and showcased stable cycling performance. Ex-situ characterizations unveiled the Mg(2+) storage mechanism of Mn-NVO involving initial extraction of Na(+) followed by subsequent Mg(2+) intercalation/deintercalation. Detailed spectroscopic analyses illuminated the formation of a pivotal solid-electrolyte interphase on the anode surface. Moreover, the solid-electrolyte interphase demonstrated a dynamic adsorption/desorption behavior, referred to as the "breathing effect", which substantially mitigated undesired dissolution and side reactions of electrode materials. These findings underscore the crucial role of rational electrolyte design in fostering the development of a favorable solid-electrolyte interphase that can significantly enhance compatibility between electrode materials and electrolytes, thus propelling advancements in aqueous multivalent-ion batteries. FAU - Song, Xinmei AU - Song X AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Ge, Yang AU - Ge Y AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Xu, Hao AU - Xu H AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Bao, Songsong AU - Bao S AUID- ORCID: 0000-0001-6770-8802 AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Wang, Lei AU - Wang L AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Xue, Xiaolan AU - Xue X AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Yu, Qianchuan AU - Yu Q AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Xing, Yizhi AU - Xing Y AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Wu, Zuoao AU - Wu Z AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Xie, Kefeng AU - Xie K AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Zhu, Tangsong AU - Zhu T AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Zhang, Pengbo AU - Zhang P AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Liu, Yuzhu AU - Liu Y AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Wang, Zhangjian AU - Wang Z AD - Jiangsu BTR Nano Technology Co., Ltd., 519 Jiangdong Avenue, Jintan District, Changzhou, Jiangsu 213200, P. R. China. FAU - Tie, Zuoxiu AU - Tie Z AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Ma, Jing AU - Ma J AUID- ORCID: 0000-0001-5848-9775 AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. FAU - Jin, Zhong AU - Jin Z AUID- ORCID: 0000-0001-8860-8579 AD - State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, China. LA - eng PT - Journal Article DEP - 20240227 PL - United States TA - J Am Chem Soc JT - Journal of the American Chemical Society JID - 7503056 SB - IM EDAT- 2024/02/27 18:42 MHDA- 2024/02/27 18:43 CRDT- 2024/02/27 17:12 PHST- 2024/02/27 18:43 [medline] PHST- 2024/02/27 18:42 [pubmed] PHST- 2024/02/27 17:12 [entrez] AID - 10.1021/jacs.4c00227 [doi] PST - ppublish SO - J Am Chem Soc. 2024 Mar 13;146(10):7018-7028. doi: 10.1021/jacs.4c00227. Epub 2024 Feb 27.