Adaptive Ionization-Induced Tunable Electric Double Layer for Practical Zn Metal Batteries over Wide pH and Temperature Ranges

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Chuyuan Lin - , Fujian Normal University (Author)
  • Lingjun He - , Fujian Normal University (Author)
  • Peixun Xiong - , TUD Dresden University of Technology (Author)
  • Hui Lin - , Fujian Normal University (Author)
  • Wenbin Lai - , Fujian Normal University (Author)
  • Xuhui Yang - , Fujian Normal University (Author)
  • Fuyu Xiao - , Fujian Normal University (Author)
  • Xiao Li Sun - , Fujian Normal University (Author)
  • Qingrong Qian - , Fujian Normal University, Nankai University (Author)
  • Shude Liu - , National Institute for Materials Science Tsukuba, Donghua University (Author)
  • Qinghua Chen - , Fujian Normal University, Nankai University (Author)
  • Stefan Kaskel - , Chair of Inorganic Chemistry I (Author)
  • Lingxing Zeng - , Fujian Normal University, Nankai University (Author)

Abstract

The violent side reactions of Zn metal in aqueous electrolyte lead to sharp local-pH fluctuations at the interface, which accelerate Zn anode breakdown; thus, the development of an optimization strategy to accommodate a wide pH range is particularly critical for improving aqueous Zn metal batteries. Herein, we report a pH-adaptive electric double layer (EDL) tuned by glycine (Gly) additive with pH-dependent ionization, which exhibits excellent capability to stabilize Zn anodes in wide-pH aqueous electrolytes. It is discovered that a Gly-ionic EDL facilitates the directed migration of charge carriers in both mildly acidic and alkaline electrolytes, leading to the successful suppression of local saturation. It is worth mentioning that the regulation effect of the additive concentration on the inner Helmholtz plane (IHP) structure of Zn electrodes is clarified in depth. It is revealed that the Gly additives without dimerization can develop orderly and dense vertical adsorption within the IHP to effectively reduce the EDL repulsive force of Zn2+ and isolate H2O from the anode surface. Consequently, they Zn anode with tunable EDL exhibits superior electrochemical performance in a wide range of pH and temperature, involving the prodigious cycle reversibility of 7000 h at Zn symmetric cells with ZnSO4-Gly electrolytes and an extended lifespan of 50 times in Zn symmetric cells with KOH-Gly electrolytes. Moreover, acidic Zn powder||MnO2 pouch cells, and alkaline high-voltage Zn||Ni0.8Co0.1Mn0.1O2 cells, and Zn||NiCo-LDH cells also deliver excellent cycling reversibility. The tunable EDL enables the ultrahigh depth of discharge (DOD) of 93%. This work elucidates the design of electrolyte additives compatible in a wide range of pH and temperature, which might cause inspiration in the fields of practical multiapplication scenarios for Zn anodes.

Details

Original languageEnglish
Pages (from-to)23181-23193
Number of pages13
JournalACS nano
Volume17
Issue number22
Publication statusPublished - 28 Nov 2023
Peer-reviewedYes

External IDs

PubMed 37956093

Keywords

Keywords

  • glycine-ionic electric double layer, pH-adaptive, wide pH range, wide temperature range, Zn metal batteries