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Title: Stable Cycling of Mg Metal Anodes by Regulating the Reactivity of Mg2+ Solvation Species

Journal Article · · Advanced Energy Materials
 [1]; ORCiD logo [2];  [2]; ORCiD logo [2];  [2]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]
  1. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Purdue Univ., West Lafayette, IN (United States)
  2. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  3. Purdue Univ., West Lafayette, IN (United States)
+ Show Author Affiliations

Rationally designing stable nonaqueous electrolytes for Mg metal anodes demands a thorough understanding of their interfacial behaviors. Here, the critical role of cation–anion pairing in improving the cathodic stabilities of amine-based electrolytes against solvent reduction and H2 evolution is identified. It is demonstrated that strong coordination between solvating amine groups and the Mg2+ cation facilitates the dehydrogenation of the -NH2 group, which is mainly responsible for low reversibility during Mg metal plating and stripping. Introducing ion-pairing into the primary solvation shell can effectively weaken the amine coordination such that its reduction is suppressed. A novel interfacial behavior regarding parasitic reaction product dissolution is also identified, which is responsible for the failure of interfacial passivation. An ion-pairing electrolyte is developed based on a weakly-solvated amine molecule and strongly coordinating Mg2+ salt. This electrolyte composition delivers long-term Mg metal anode cycling with 99.6% Coulombic efficiency for 800 cycles.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
2407056
Report Number(s):
PNNL-SA--195286
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 16 Vol. 14; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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