TY - JOUR
T1 - Highly reversible Zn metal anode enabled by sustainable hydroxyl chemistry
AU - Ma, Lin
AU - Vatamanu, Jenel
AU - Hahn, Nathan T.
AU - Pollard, Travis P.
AU - Borodin, Oleg
AU - Petkov, Valeri
AU - Schroeder, Marshall A.
AU - Ren, Yang
AU - Ding, Michael S.
AU - Luo, Chao
AU - Allen, Jan L.
AU - Wang, Chunsheng
AU - Xu, Kang
N1 - Funding Information:
ACKNOWLEDGMENTS. This work was supported by the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the US Department of Energy (DOE), through IAA SN2020957. L.M. also acknowledges the Army Research Laboratory for providing financial support under the Dr. Brad. E. Forch Distinguished Postdoctoral Fellowship administered by the National Research Council. This research used resources of the Advanced Photon Source, a DOE Office of Science User Facility, operated for the DOE Office of Science by Argonne National Laboratory under contract number DE-AC02-06CH11357. C.L. acknowledges support from the George Mason University Quantum Science & Engineering Center. The authors thank Dr. Jiancun Rao and Dr. Sz-Chian Liou (Advanced Imaging & Microscopy Laboratory in the University of Maryland) for TEM assistance. The authors thank Dr. Jeff Read (US Army Research Laboratory), Dr. Shengshui Zhang (US Army Research Laboratory), and Professor Nitash P. Bal-sara (University of California, Berkeley) for useful discussions and guidance. The help of Jean-Philip Piquemal and Louis Lagardere (Sorbonne Université) with Tinker-HP installation and modification is acknowledged. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the DOE’s National Nuclear Security Administration under contract DE-NA0003525. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the DOE or the US government.
Publisher Copyright:
Copyright © 2022 the Author(s).
PY - 2022/6/14
Y1 - 2022/6/14
N2 - Rechargeable Zn metal batteries (RZMBs) may provide a more sustainable and lower-cost alternative to established battery technologies in meeting energy storage applications of the future. However, the most promising electrolytes for RZMBs are generally aqueous and require high concentrations of salt(s) to bring efficiencies toward commercially viable levels and mitigate water-originated parasitic reactions including hydrogen evolution and corrosion. Electrolytes based on nonaqueous solvents are promising for avoiding these issues, but full cell performance demonstrations with solvents other than water have been very limited. To address these challenges, we investigated MeOH as an alternative electrolyte solvent. These MeOH-based electrolytes exhibited exceptional Zn reversibility over a wide temperature range, with a Coulombic efficiency > 99.5% at 50% Zn utilization without cell short-circuit behavior for > 1,800 h. More important, this remarkable performance translates well to Zn jj metal-free organic cathode full cells, supporting < 6% capacity decay after > 800 cycles at 240 °C.
AB - Rechargeable Zn metal batteries (RZMBs) may provide a more sustainable and lower-cost alternative to established battery technologies in meeting energy storage applications of the future. However, the most promising electrolytes for RZMBs are generally aqueous and require high concentrations of salt(s) to bring efficiencies toward commercially viable levels and mitigate water-originated parasitic reactions including hydrogen evolution and corrosion. Electrolytes based on nonaqueous solvents are promising for avoiding these issues, but full cell performance demonstrations with solvents other than water have been very limited. To address these challenges, we investigated MeOH as an alternative electrolyte solvent. These MeOH-based electrolytes exhibited exceptional Zn reversibility over a wide temperature range, with a Coulombic efficiency > 99.5% at 50% Zn utilization without cell short-circuit behavior for > 1,800 h. More important, this remarkable performance translates well to Zn jj metal-free organic cathode full cells, supporting < 6% capacity decay after > 800 cycles at 240 °C.
KW - Zn metal batteries
KW - high reversibility
KW - solid electrolyte interphase
KW - sustainable electrolyte design
UR - http://www.scopus.com/inward/record.url?scp=85131627563&partnerID=8YFLogxK
U2 - 10.1073/pnas.2121138119
DO - 10.1073/pnas.2121138119
M3 - Article
C2 - 35675422
AN - SCOPUS:85131627563
SN - 0027-8424
VL - 119
JO - Proceedings of the National Academy of Sciences of the United States of America
JF - Proceedings of the National Academy of Sciences of the United States of America
IS - 24
M1 - e2121138119
ER -