Superhalide-Anion-Motivator Reforming-Enabled Bipolar Manipulation toward Longevous Energy-Type Zn||Chalcogen Batteries

Hongqing Li; Jintu Qi; Yongchao Tang; Guigui Liu; Jianping Yan; Zhenfeng Feng; Yue Wei; Qi Yang; Minghui Ye; Yufei Zhang; Zhipeng Wen; Xiaoqing Liu; Cheng Chao Li

doi:10.1021/acs.nanolett.4c00198

Superhalide-Anion-Motivator Reforming-Enabled Bipolar Manipulation toward Longevous Energy-Type Zn||Chalcogen Batteries

Nano Lett. 2024 Jun 5;24(22):6465-6473. doi: 10.1021/acs.nanolett.4c00198. Epub 2024 May 20.

Authors

Hongqing Li¹, Jintu Qi¹, Yongchao Tang^{1

2}, Guigui Liu¹, Jianping Yan¹, Zhenfeng Feng¹, Yue Wei³, Qi Yang⁴, Minghui Ye¹, Yufei Zhang¹, Zhipeng Wen¹, Xiaoqing Liu¹, Cheng Chao Li^{1

2}

Affiliations

¹ School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China.
² Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, China.
³ School of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, 523808 Guangdong China.
⁴ State Key Laboratory of Chemical Resource Engineering, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China.

PMID: 38767853
DOI: 10.1021/acs.nanolett.4c00198

Abstract

Neutrophilic superhalide-anion-triggered chalcogen conversion-based Zn batteries, despite latent high-energy merit, usually suffer from a short lifespan caused by dendrite growth and shuttle effect. Here, a superhalide-anion-motivator reforming strategy is initiated to simultaneously manipulate the anode interface and Se conversion intermediates, realizing a bipolar regulation toward longevous energy-type Zn batteries. With ZnF₂ chaotropic additives, the original large-radii superhalide zincate anion species in ionic liquid (IL) electrolytes are split into small F-containing species, boosting the formation of robust solid electrolyte interphases (SEI) for Zn dendrite inhibition. Simultaneously, ion radius reduced multiple F-containing Se conversion intermediates form, enhancing the interion interaction of charged products to suppress the shuttle effect. Consequently, Zn||Se batteries deliver a ca. 20-fold prolonged lifespan (2000 cycles) at 1 A g^-1 and high energy/power density of 416.7 Wh kg_Se^-1/1.89 kW kg_Se^-1, outperforming those in F-free counterparts. Pouch cells with distinct plateaus and durable cyclability further substantiate the practicality of this design.

Keywords: Se conversion intermediates; Zn||chalcogen batteries; bipolar manipulation; solid electrolyte interphase; superhalide-anion-motivator reforming.