Mechanistic Insights into the Interplay between Ion Intercalation and Water Electrolysis in Aqueous Batteries

Yuxin Zhang, Chunguang Kuai, Anyang Hu, Lu Ma, Sha Tan, Inhui Hwang, Linqin Mu, Muhammad Mominur Rahman, Cheng Jun Sun, Luxi Li, Enyuan Hu, Feng Lin

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Improving electrolyte stability to suppress water electrolysis represents a basic principle for designing aqueous batteries. Herein, we investigate counterintuitive roles that water electrolysis plays in regulating intercalation chemistry. Using the NaxFe[Fe(CN)6]∥NaTi2(PO4)3 (x < 1) aqueous battery as a platform, we report that high-voltage overcharging can serve as an electrochemical activation approach to achieving concurrent Na-ion intercalation and an electrolytic oxygen evolution reaction. When the cell capacity is intrinsically limited by deficient cyclable Na ions, the electrolytic water oxidation on the cathode allows for extra Na-ion intercalation from the electrolyte to the NaTi2(PO4)3 anode, leading to a major increase in cyclable Na ions and specific capacity. The parasitic oxygen generation and potential transition-metal dissolution, as proved by our synchrotron and imaging tools, can be significantly mitigated with a simple reassembling approach, which enables stable electrochemical performance and sheds light on manipulating ion intercalation and water electrolysis for battery fast charging and recycling.

Original languageEnglish
Pages (from-to)12130-12139
Number of pages10
JournalACS Applied Materials and Interfaces
Volume14
Issue number10
DOIs
StatePublished - Mar 16 2022
Externally publishedYes

Funding

The project was supported by the National Science Foundation (No. CBET-1912885). The use of the Stanford Synchrotron Radiation Light source, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract no. DE-AC02-76SF00515. S.T. and E.H. at Brookhaven National Laboratory (BNL) were supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program, under contract DE-SC0012704. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract no. DE-AC02-06CH11357.

Keywords

  • aqueous battery
  • electrochemical activation
  • electrolytic reaction
  • fast charging
  • ion intercalation

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