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Decoupled aqueous batteries using pH-decoupling electrolytes

Nature Reviews Chemistry volume 6, pages 505–517 (2022)Cite this article

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Abstract

Aqueous batteries have been considered as the most promising alternatives to the dominant lithium-based battery technologies because of their low cost, abundant resources and high safety. The output voltage of aqueous batteries is limited by the narrow stable voltage window of 1.23 V for water, which theoretically impedes further improvement of their energy density. However, the pH-decoupling electrolyte with an acidic catholyte and an alkaline anolyte has been verified to broaden the operating voltage window of the aqueous electrolyte to over 3 V, which goes beyond the voltage limitations of the aqueous batteries, making high-energy aqueous batteries possible. In this Review, we summarize the latest decoupled aqueous batteries based on pH-decoupling electrolytes from the perspective of ion-selective membranes, competitive redox couples and potential battery prototypes. The inherent defects and problems of these decoupled aqueous batteries are systematically analysed, and the critical scientific issues of this battery technology for future applications are discussed.

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Fig. 1: Typical strategies for widening the operating voltage window of aqueous electrolytes.
Fig. 2: Ion-selective membrane in a decoupled battery.
Fig. 3: Liquid junction potential in a decoupled battery.
Fig. 4: Redox couples in a decoupled battery.
Fig. 5: Decoupled battery prototypes.
Fig. 6: Cell configurations for decoupled batteries in the future.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (grant nos. 21725103, 51522101, 51471075, 51631004 and 51401084), National Key R&D Program of China (grant no. 2019YFA0705700) and the China Postdoctoral Science Foundation (grant no. 2020M681035).

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  1. State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, China

    Yun-hai Zhu, Yang-feng Cui, Zi-long Xie, Zhen-bang Zhuang, Gang Huang & Xin-bo Zhang

  2. Key Laboratory of Automobile Materials (Jilin University), Ministry of Education, Department of Materials Science and Engineering, Jilin University, Changchun, China

    Yun-hai Zhu & Zhen-bang Zhuang

  3. School of Materials Science and Engineering, Changchun University of Science and Technology, Changchun, China

    Yang-feng Cui

  4. University of Science and Technology of China, Hefei, China

    Zi-long Xie & Xin-bo Zhang

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X.Z. and Y.Z. contributed to the writing and editing of all sections of the manuscript. All authors contributed to the research and discussion of data, figure preparation and proofreading of the manuscript.

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Glossary

Ion-selective membrane

(ISM). A semipermeable membrane that has selective transmissibility to specific ions in solution.

Permselectivity

A term to define the preferential permeation of certain ionic species through ion-exchange membranes.

Donnan equilibrium

Also known as the Gibbs–Donnan effect, the behaviour of charged particles near a semipermeable membrane, which sometimes fail to distribute evenly across the two sides of the membrane.

Bipolar membranes

(BPMs). A special class of ion-exchange membranes constituted by a cation-exchange and an anion-exchange layer, which allows the generation of protons and hydroxide ions via a water dissociation mechanism.

Proton-exchange membrane

(PEM). A kind of semipermeable membrane generally made from ionomers and designed to conduct protons.

Grotthuss mechanism

Also known as proton-hopping mechanism, a proton transport mode in the hydrogen-bond network of water molecules or other hydrogen-bonded liquids, which is completed via the cooperative breaking and formation of hydrogen bonds and O–H covalent bonds.

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Zhu, Yh., Cui, Yf., Xie, Zl. et al. Decoupled aqueous batteries using pH-decoupling electrolytes. Nat Rev Chem 6, 505–517 (2022). https://doi.org/10.1038/s41570-022-00397-3

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