Decoupling, quantifying, and restoring aging-induced Zn-anode losses in rechargeable aqueous zinc batteries

Shengda D. Pu; Bingkun Hu; Zixuan Li; Yi Yuan; Chen Gong; Ziyang Ning; Chloe Chau; Sixie Yang; Shengming Zhang; Liquan Pi; Yuanbo T. Tang; Jili Yue; T. James Marrow; Xiangwen Gao; Peter G. Bruce; Alex W. Robertson

doi:10.1016/j.joule.2023.01.010

Decoupling, quantifying, and restoring aging-induced Zn-anode losses in rechargeable aqueous zinc batteries

Shengda D. Pu^*, Bingkun Hu, Zixuan Li, Yi Yuan, Chen Gong, Ziyang Ning, Chloe Chau, Sixie Yang, Shengming Zhang, Liquan Pi, Yuanbo T. Tang, Jili Yue, T. James Marrow, Xiangwen Gao^*, Peter G. Bruce^*, Alex W. Robertson^*

^*Corresponding author for this work

Metallurgy and Materials

Research output: Contribution to journal › Article › peer-review

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Abstract

Rechargeable aqueous zinc batteries offer low cost, safety, and good cycling capacity, largely due to the water-compatible Zn-metal anode. However, Zn anodes corrode in aqueous electrolytes. While such corrosion is well known, distinguishing the relative importance of corrosion contributions toward anode capacity loss remains less understood. Here, by systematically cycling Zn anodes with controlled loading and under different aging conditions, we successfully decouple and quantify the aging-induced contributions toward anode degradation in mildly acidic aqueous electrolytes. While some losses occur due to the irreversible consumption of Zn into corrosion by-products, we demonstrate that the bigger contributor to this efficiency loss (over 80%) is the physical screening effect of evolved gases, preventing the reversible dissolution of deposited Zn. Understanding the crucial role of evolved gas during cell aging, and how it can accumulate and effectively passivate large sections of the battery anode, will have important implications in the development of rechargeable aqueous zinc batteries.

Original language	English
Pages (from-to)	366-379
Number of pages	14
Journal	Joule
Volume	7
Issue number	2
DOIs	https://doi.org/10.1016/j.joule.2023.01.010
Publication status	Published - 15 Feb 2023

Bibliographical note

Acknowledgments:
The authors thank the support and acknowledge the use of the facilities of the DCCEM, at the Materials Department, Oxford (EP/R010145/1). P.G.B. is indebted to the Engineering and Physical Sciences Research Council (EPSRC), including the SUPERGEN Energy Storage Hub (EP/L019469/1), Enabling Next Generation Lithium Batteries (EP/M009521/1), Henry Royce Institute for Advanced Materials, and the Faraday for financial support. A.W.R. thanks the support of the Royal Society (UF160183). The XCT was facilitated by EPSRC grant EP/M02833X/1. The Zeiss Crossbeam FIB/SEM was supported by EPSRC grant EP/N010868/1.

Keywords

rechargeable aqueous zinc battery
zinc-metal anode
corrosion

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title = "Decoupling, quantifying, and restoring aging-induced Zn-anode losses in rechargeable aqueous zinc batteries",

abstract = "Rechargeable aqueous zinc batteries offer low cost, safety, and good cycling capacity, largely due to the water-compatible Zn-metal anode. However, Zn anodes corrode in aqueous electrolytes. While such corrosion is well known, distinguishing the relative importance of corrosion contributions toward anode capacity loss remains less understood. Here, by systematically cycling Zn anodes with controlled loading and under different aging conditions, we successfully decouple and quantify the aging-induced contributions toward anode degradation in mildly acidic aqueous electrolytes. While some losses occur due to the irreversible consumption of Zn into corrosion by-products, we demonstrate that the bigger contributor to this efficiency loss (over 80%) is the physical screening effect of evolved gases, preventing the reversible dissolution of deposited Zn. Understanding the crucial role of evolved gas during cell aging, and how it can accumulate and effectively passivate large sections of the battery anode, will have important implications in the development of rechargeable aqueous zinc batteries.",

keywords = "rechargeable aqueous zinc battery, zinc-metal anode, corrosion",

author = "Pu, {Shengda D.} and Bingkun Hu and Zixuan Li and Yi Yuan and Chen Gong and Ziyang Ning and Chloe Chau and Sixie Yang and Shengming Zhang and Liquan Pi and Tang, {Yuanbo T.} and Jili Yue and Marrow, {T. James} and Xiangwen Gao and Bruce, {Peter G.} and Robertson, {Alex W.}",

note = "Acknowledgments: The authors thank the support and acknowledge the use of the facilities of the DCCEM, at the Materials Department, Oxford (EP/R010145/1). P.G.B. is indebted to the Engineering and Physical Sciences Research Council (EPSRC), including the SUPERGEN Energy Storage Hub (EP/L019469/1), Enabling Next Generation Lithium Batteries (EP/M009521/1), Henry Royce Institute for Advanced Materials, and the Faraday for financial support. A.W.R. thanks the support of the Royal Society (UF160183). The XCT was facilitated by EPSRC grant EP/M02833X/1. The Zeiss Crossbeam FIB/SEM was supported by EPSRC grant EP/N010868/1.",

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T1 - Decoupling, quantifying, and restoring aging-induced Zn-anode losses in rechargeable aqueous zinc batteries

AU - Pu, Shengda D.

AU - Hu, Bingkun

AU - Li, Zixuan

AU - Yuan, Yi

AU - Gong, Chen

AU - Ning, Ziyang

AU - Chau, Chloe

AU - Yang, Sixie

AU - Zhang, Shengming

AU - Pi, Liquan

AU - Tang, Yuanbo T.

AU - Yue, Jili

AU - Marrow, T. James

AU - Gao, Xiangwen

AU - Bruce, Peter G.

AU - Robertson, Alex W.

N1 - Acknowledgments: The authors thank the support and acknowledge the use of the facilities of the DCCEM, at the Materials Department, Oxford (EP/R010145/1). P.G.B. is indebted to the Engineering and Physical Sciences Research Council (EPSRC), including the SUPERGEN Energy Storage Hub (EP/L019469/1), Enabling Next Generation Lithium Batteries (EP/M009521/1), Henry Royce Institute for Advanced Materials, and the Faraday for financial support. A.W.R. thanks the support of the Royal Society (UF160183). The XCT was facilitated by EPSRC grant EP/M02833X/1. The Zeiss Crossbeam FIB/SEM was supported by EPSRC grant EP/N010868/1.

PY - 2023/2/15

Y1 - 2023/2/15

N2 - Rechargeable aqueous zinc batteries offer low cost, safety, and good cycling capacity, largely due to the water-compatible Zn-metal anode. However, Zn anodes corrode in aqueous electrolytes. While such corrosion is well known, distinguishing the relative importance of corrosion contributions toward anode capacity loss remains less understood. Here, by systematically cycling Zn anodes with controlled loading and under different aging conditions, we successfully decouple and quantify the aging-induced contributions toward anode degradation in mildly acidic aqueous electrolytes. While some losses occur due to the irreversible consumption of Zn into corrosion by-products, we demonstrate that the bigger contributor to this efficiency loss (over 80%) is the physical screening effect of evolved gases, preventing the reversible dissolution of deposited Zn. Understanding the crucial role of evolved gas during cell aging, and how it can accumulate and effectively passivate large sections of the battery anode, will have important implications in the development of rechargeable aqueous zinc batteries.

AB - Rechargeable aqueous zinc batteries offer low cost, safety, and good cycling capacity, largely due to the water-compatible Zn-metal anode. However, Zn anodes corrode in aqueous electrolytes. While such corrosion is well known, distinguishing the relative importance of corrosion contributions toward anode capacity loss remains less understood. Here, by systematically cycling Zn anodes with controlled loading and under different aging conditions, we successfully decouple and quantify the aging-induced contributions toward anode degradation in mildly acidic aqueous electrolytes. While some losses occur due to the irreversible consumption of Zn into corrosion by-products, we demonstrate that the bigger contributor to this efficiency loss (over 80%) is the physical screening effect of evolved gases, preventing the reversible dissolution of deposited Zn. Understanding the crucial role of evolved gas during cell aging, and how it can accumulate and effectively passivate large sections of the battery anode, will have important implications in the development of rechargeable aqueous zinc batteries.

KW - rechargeable aqueous zinc battery

KW - zinc-metal anode

KW - corrosion

U2 - 10.1016/j.joule.2023.01.010

DO - 10.1016/j.joule.2023.01.010

M3 - Article

SN - 2542-4351

VL - 7

SP - 366

EP - 379

JO - Joule

JF - Joule

IS - 2

ER -

Decoupling, quantifying, and restoring aging-induced Zn-anode losses in rechargeable aqueous zinc batteries

Abstract

Bibliographical note

Keywords

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