Theory-Driven Design of a Cationic Accelerator for High-Performance Electrolytic MnO2 -Zn Batteries

Mingyan Chuai; Jinlong Yang; Rui Tan; Zaichun Liu; Yuan Yuan; Yan Xu; Jifei Sun; Mingming Wang; Xinhua Zheng; Na Chen; Wei Chen

doi:10.1002/adma.202203249

Theory-Driven Design of a Cationic Accelerator for High-Performance Electrolytic MnO₂ -Zn Batteries

Adv Mater. 2022 Aug;34(33):e2203249. doi: 10.1002/adma.202203249. Epub 2022 Jul 20.

Authors

Mingyan Chuai^{1

2}, Jinlong Yang¹, Rui Tan³, Zaichun Liu^{1

2}, Yuan Yuan^{1

2}, Yan Xu², Jifei Sun², Mingming Wang², Xinhua Zheng², Na Chen², Wei Chen²

Affiliations

¹ Guangdong Research Center for Interfacial Engineering of Functional Materials, College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518060, China.
² Department of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, China.
³ Department of Chemical Engineering, Imperial College London, London, SW72AZ, UK.

PMID: 35766725
DOI: 10.1002/adma.202203249

Abstract

Aqueous electrolytic MnO₂ -Zn batteries are considered as one of the most promising energy-storage devices for their cost effectiveness, high output voltage, and safety, but their electrochemical performance is limited by the sluggish kinetics of cathodic MnO₂ /Mn²⁺ and anodic Zn/Zn²⁺ reactions. To overcome this critical challenge, herein, a cationic accelerator (CA) strategy is proposed based on the prediction of first-principles calculations. Poly(vinylpyrrolidone) is utilized as a model to testify the rational design of the CA strategy. It manifests that the CA effectively facilitates rapid cations migration in electrolyte and adequate charge transfer at electrode-electrolyte interface, benefiting the deposition/dissolution processes of both Mn²⁺ and Zn²⁺ cations to simultaneously improve kinetics of cathodic MnO₂ /Mn²⁺ and anodic Zn/Zn²⁺ reactions. The resulting MnO₂ -Zn battery regulated by CA exhibits large reversible capacities of 455 mAh g^-1 and 3.64 mAh cm^-2 at 20 C, as well as a long lifespan of 2000 cycles with energy density retention of 90%, achieving one of the best overall performances in the electrolytic MnO₂ -Zn batteries. This comprehensive work integrating theoretical prediction with experimental studies provides opportunities to the development of high-performance energy-storage devices.

Keywords: cation migration; cationic accelerators; deposition/dissolution chemistry; electrolytic MnO 2-Zn batteries; large-scale energy storage.

Abstract

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