4.8 Article

A Carboranyl Electrolyte Enabling Highly Reversible Sodium Metal Anodes via a Fluorine-Free SEI

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 51, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202208158

Keywords

Anode-Free Batteries; Carboranes; Electrochemistry; Electrolyte Engineering; Sodium Metal Anodes

Funding

  1. U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program
  2. ORAU [DE-SC0014664]
  3. Advanced Battery Materials Research (BMR) Program
  4. U.S. Department of Energy Office of Science Laboratory [DE-AC02-06CH11357]
  5. Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences
  6. DOE Office of Science [AC02-06CH11357]
  7. NSF [DMR-2004497]

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This article presents advanced characterization of a novel fluorine-free electrolyte for sodium metal batteries. The electrolyte enables low overpotential and high coulombic efficiency in Na cell operation. The study identifies weak ion-pairing as key for the successful development of fluorine-free sodium electrolytes.
Realization of practical sodium metal batteries (SMBs) is hindered due to lack of compatible electrolyte components, dendrite propagation, and poor understanding of anodic interphasial chemistries. Chemically robust liquid electrolytes that facilitate both favorable sodium metal deposition and a stable solid-electrolyte interphase (SEI) are ideal to enable sodium metal and anode-free cells. Herein we present advanced characterization of a novel fluorine-free electrolyte utilizing the [HCB11H11](1-) anion. Symmetrical Na cells operated with this electrolyte exhibit a remarkably low overpotential of 0.032 V at a current density of 2.0 mA cm(-2) and a high coulombic efficiency of 99.5 % in half-cell configurations. Surface characterization of electrodes post-operation reveals the absence of dendritic sodium nucleation and a surprisingly stable fluorine-free SEI. Furthermore, weak ion-pairing is identified as key towards the successful development of fluorine-free sodium electrolytes.

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