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

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

doi:10.1021/acsami.1c19684

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

Journal Article · 28 February 2022 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.1c19684 · OSTI ID:1867199

^[1]; Kuai, Chunguang ^[1];

^[1]; Ma, Lu ^[2]; Tan, Sha ^[2]; Hwang, Inhui ^[3];

^[1];

^[1]; Sun, Cheng-Jun ^[3]; Li, Luxi ^[3];

^[2];

^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

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 Na_xFe[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. Furthermore, 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; SC0012704

OSTI ID:: 1867199

Report Number(s):: BNL-222961-2022-JAAM

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 10 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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