Title: Tuning the Solvation Structure in Aqueous Zinc Batteries to Maximize Zn-Ion Intercalation and Optimize Dendrite-Free Zinc Plating

Journal Article · · ACS Energy Letters
 [1];  [2]; ORCiD logo [1];  [1]; ORCiD logo [3]; ORCiD logo [1]
  1. University of Waterloo, ON (Canada); Argonne National Laboratory (ANL), Lemont, IL (United States). Joint Center for Energy Storage Research (JCESR)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
+ Show Author Affiliations

Aqueous zinc batteries are recognized to suffer from H+/Zn2+ coinsertion in the cathode, but few approaches have been reported to suppress deleterious H+ intercalation. We realize this goal by tuning the solvation structure, using LiV2(PO4)3 (LVP) as a model cathode. Phase conversion of LVP induced by H+ intercalation is observed in 4 m Zn(OTf)2, whereas dominant Zn2+ insertion is confirmed in a ZnCl2 water-in-salt electrolyte (WiSE). This disparity is ascribed to the complete absence of free water and a strong Zn2+–H2O interaction in the latter that interrupts the H2O hydrogen bonding network, thus suppressing H+ intercalation. On the basis of this strategy, a novel PEG-based hybrid electrolyte is designed to replace the corrosive ZnCl2 WiSE. This system exhibits an optimized Zn2+ solvation sheath with a similar low free water content, showing not only much better suppression of H+ intercalation but also highly reversible Zn plating/stripping with a CE of ~99.7% over 150 cycles.

Research Organization:
Argonne National Laboratory (ANL), Lemont, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
Discovery Grant and Canada Research Chair; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1963433
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 1 Vol. 7; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (25)

ZnCl 2 “Water‐in‐Salt” Electrolyte Transforms the Performance of Vanadium Oxide as a Zn Battery Cathode journal May 2019
Stabilizing Zinc Anode Reactions by Polyethylene Oxide Polymer in Mild Aqueous Electrolytes journal September 2020
Quantifying and Suppressing Proton Intercalation to Enable High‐Voltage Zn‐Ion Batteries journal October 2021
Inhibiting VOPO 4 ⋅ x  H 2 O Decomposition and Dissolution in Rechargeable Aqueous Zinc Batteries to Promote Voltage and Capacity Stabilities journal November 2019
Surface Adsorption of Polyethylene Glycol to Suppress Dendrite Formation on Zinc Anodes in Rechargeable Aqueous Batteries journal June 2018
The electrolyte comprising more robust water and superhalides transforms Zn‐metal anode reversibly and dendrite‐free journal August 2020
Polyethylene glycol aggregates in water formed through hydrophobic helical structures journal August 2012
Scientific Challenges for the Implementation of Zn-Ion Batteries journal April 2020
Manipulating Zn anode reactions through salt anion involving hydrogen bonding network in aqueous electrolytes with PEO additive journal April 2021
NASICON Na 3 V 2 (PO 4 ) 3 Enables Quasi-Two-Stage Na + and Zn 2+ Intercalation for Multivalent Zinc Batteries journal March 2020
Oxide versus Nonoxide Cathode Materials for Aqueous Zn Batteries: An Insight into the Charge Storage Mechanism and Consequences Thereof journal December 2018
Multivalent-Ion versus Proton Insertion into Battery Electrodes journal June 2020
Operando pH Measurements Decipher H + /Zn 2+ Intercalation Chemistry in High-Performance Aqueous Zn/δ-V 2 O 5 Batteries journal September 2020
Tailoring the Stability and Kinetics of Zn Anodes through Trace Organic Polymer Additives in Dilute Aqueous Electrolyte journal August 2021
Electrochemical Property:  Structure Relationships in Monoclinic Li 3 - y V 2 (PO 4 ) 3 journal August 2003
Zn/MnO 2 Battery Chemistry With H + and Zn 2+ Coinsertion journal July 2017
A high-capacity and long-life aqueous rechargeable zinc battery using a metal oxide intercalation cathode journal August 2016
Reversible aqueous zinc/manganese oxide energy storage from conversion reactions journal April 2016
Polyaniline-intercalated manganese dioxide nanolayers as a high-performance cathode material for an aqueous zinc-ion battery journal July 2018
A ZnCl 2 water-in-salt electrolyte for a reversible Zn metal anode journal January 2018
A rechargeable aqueous Zn 2+ -battery with high power density and a long cycle-life journal January 2018
Voltage issue of aqueous rechargeable metal-ion batteries journal January 2020
Structural impact of Zn-insertion into monoclinic V 2 (PO 4 ) 3 : implications for Zn-ion batteries journal January 2019
Rechargeable aqueous electrolyte batteries: from univalent to multivalent cation chemistry journal January 2019
The critical effect of water content in the electrolyte on the reversible electrochemical performance of Zn–VPO 4 F cells journal January 2020

Similar Records

Achieving Stable Molybdenum Oxide Cathodes for Aqueous Zinc-Ion Batteries in Water-in-Salt Electrolyte
Journal Article · 2021 · Advanced Materials Interfaces · OSTI ID:1778914
+7 more
Solvation Structure Design for Aqueous Zn Metal Batteries
Journal Article · 2020 · Journal of the American Chemical Society · OSTI ID:1737441
+6 more
Quantifying and Suppressing Proton Intercalation to Enable High-Voltage Zn-Ion Batteries
Journal Article · 2021 · Advanced Energy Materials · OSTI ID:1827175
+9 more

Related Subjects

25 ENERGY STORAGE
diffraction
electrodes
electrolytes
intercalation
molecules