Organic pH Buffer for Dendrite-Free and Shuttle-Free Zn-I2 Batteries

Yanqiu Lyu; Jodie A. Yuwono; Pengtang Wang; Yanyan Wang; Fuhua Yang; Sailin Liu; Shilin Zhang; Baofeng Wang; Kenneth Davey; Jianfeng Mao; Zaiping Guo

doi:10.1002/anie.202303011

Organic pH Buffer for Dendrite-Free and Shuttle-Free Zn-I₂ Batteries

Yanqiu Lyu, Jodie A. Yuwono, Pengtang Wang, Yanyan Wang, Fuhua Yang, Sailin Liu, Shilin Zhang, Baofeng Wang, Kenneth Davey, Jianfeng Mao^*, Zaiping Guo^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

216 Citations (Scopus)

Abstract

Aqueous Zn-Iodine (I₂) batteries are attractive for large-scale energy storage. However, drawbacks include, Zn dendrites, hydrogen evolution reaction (HER), corrosion and, cathode “shuttle” of polyiodines. Here we report a class of N-containing heterocyclic compounds as organic pH buffers to obviate these. We evidence that addition of pyridine /imidazole regulates electrolyte pH, and inhibits HER and anode corrosion. In addition, pyridine and imidazole preferentially absorb on Zn metal, regulating non-dendritic Zn plating /stripping, and achieving a high Coulombic efficiency of 99.6 % and long-term cycling stability of 3200 h at 2 mA cm⁻², 2 mAh cm⁻². It is also confirmed that pyridine inhibits polyiodines shuttling and boosts conversion kinetics for I⁻/I₂. As a result, the Zn-I₂ full battery exhibits long cycle stability of >25 000 cycles and high specific capacity of 105.5 mAh g⁻¹ at 10 A g⁻¹. We conclude organic pH buffer engineering is practical for dendrite-free and shuttle-free Zn-I₂ batteries. © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Original language	English
Article number	e202303011
Number of pages	10
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	21
Online published	22 Mar 2023
DOIs	https://doi.org/10.1002/anie.202303011
Publication status	Published - 15 May 2023
Externally published	Yes

Funding

Financial support provided by the Australian Research Council (ARC) Discovery Projects (DP200101862, FL210100050) is gratefully acknowledged. Open Access publishing facilitated by The University of Adelaide, as part of the Wiley - The University of Adelaide agreement via the Council of Australian University Librarians.

Research Keywords

Electrolyte Additives
Organic pH Buffer
Zn Metal
Zn−Iodine Batteries

Publisher's Copyright Statement

This full text is made available under CC-BY-NC 4.0. https://creativecommons.org/licenses/by-nc/4.0/

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "Organic pH Buffer for Dendrite-Free and Shuttle-Free Zn-I2 Batteries",

abstract = "Aqueous Zn-Iodine (I2) batteries are attractive for large-scale energy storage. However, drawbacks include, Zn dendrites, hydrogen evolution reaction (HER), corrosion and, cathode “shuttle” of polyiodines. Here we report a class of N-containing heterocyclic compounds as organic pH buffers to obviate these. We evidence that addition of pyridine /imidazole regulates electrolyte pH, and inhibits HER and anode corrosion. In addition, pyridine and imidazole preferentially absorb on Zn metal, regulating non-dendritic Zn plating /stripping, and achieving a high Coulombic efficiency of 99.6 % and long-term cycling stability of 3200 h at 2 mA cm−2, 2 mAh cm−2. It is also confirmed that pyridine inhibits polyiodines shuttling and boosts conversion kinetics for I−/I2. As a result, the Zn-I2 full battery exhibits long cycle stability of >25 000 cycles and high specific capacity of 105.5 mAh g−1 at 10 A g−1. We conclude organic pH buffer engineering is practical for dendrite-free and shuttle-free Zn-I2 batteries. {\textcopyright} 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

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author = "Yanqiu Lyu and Yuwono, {Jodie A.} and Pengtang Wang and Yanyan Wang and Fuhua Yang and Sailin Liu and Shilin Zhang and Baofeng Wang and Kenneth Davey and Jianfeng Mao and Zaiping Guo",

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T1 - Organic pH Buffer for Dendrite-Free and Shuttle-Free Zn-I2 Batteries

AU - Lyu, Yanqiu

AU - Yuwono, Jodie A.

AU - Wang, Pengtang

AU - Wang, Yanyan

AU - Yang, Fuhua

AU - Liu, Sailin

AU - Zhang, Shilin

AU - Wang, Baofeng

AU - Davey, Kenneth

AU - Mao, Jianfeng

AU - Guo, Zaiping

PY - 2023/5/15

Y1 - 2023/5/15

N2 - Aqueous Zn-Iodine (I2) batteries are attractive for large-scale energy storage. However, drawbacks include, Zn dendrites, hydrogen evolution reaction (HER), corrosion and, cathode “shuttle” of polyiodines. Here we report a class of N-containing heterocyclic compounds as organic pH buffers to obviate these. We evidence that addition of pyridine /imidazole regulates electrolyte pH, and inhibits HER and anode corrosion. In addition, pyridine and imidazole preferentially absorb on Zn metal, regulating non-dendritic Zn plating /stripping, and achieving a high Coulombic efficiency of 99.6 % and long-term cycling stability of 3200 h at 2 mA cm−2, 2 mAh cm−2. It is also confirmed that pyridine inhibits polyiodines shuttling and boosts conversion kinetics for I−/I2. As a result, the Zn-I2 full battery exhibits long cycle stability of >25 000 cycles and high specific capacity of 105.5 mAh g−1 at 10 A g−1. We conclude organic pH buffer engineering is practical for dendrite-free and shuttle-free Zn-I2 batteries. © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

AB - Aqueous Zn-Iodine (I2) batteries are attractive for large-scale energy storage. However, drawbacks include, Zn dendrites, hydrogen evolution reaction (HER), corrosion and, cathode “shuttle” of polyiodines. Here we report a class of N-containing heterocyclic compounds as organic pH buffers to obviate these. We evidence that addition of pyridine /imidazole regulates electrolyte pH, and inhibits HER and anode corrosion. In addition, pyridine and imidazole preferentially absorb on Zn metal, regulating non-dendritic Zn plating /stripping, and achieving a high Coulombic efficiency of 99.6 % and long-term cycling stability of 3200 h at 2 mA cm−2, 2 mAh cm−2. It is also confirmed that pyridine inhibits polyiodines shuttling and boosts conversion kinetics for I−/I2. As a result, the Zn-I2 full battery exhibits long cycle stability of >25 000 cycles and high specific capacity of 105.5 mAh g−1 at 10 A g−1. We conclude organic pH buffer engineering is practical for dendrite-free and shuttle-free Zn-I2 batteries. © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

KW - Electrolyte Additives

KW - Organic pH Buffer

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