Advanced Materials

Binary Electrolyte Additive‐Reinforced Interfacial Molecule Adsorption Layer for Ultra‐Stable Zinc Metal Anodes

Kai Liu 1
Mingzi Sun 2, 3
Yan Wu 4
Tian Zhang 1
Anquan Zhu 1
Shuyu Bu 1
Chuhao Luan 1
Kunlun Liu 1
Yin Zhou 1
Dewu Lin 1
Shuilin Wu 5
Chun Sing Lee 4
Bolong Huang 2, 3
Guo Hong 1, 6
Wenjun Zhang 1
Show full list: 15 authors
1
 
Department of Materials Science and Engineering and Center of Super‐Diamond and Advanced Films (COSDAF) City University of Hong Kong 83 Tat Chee Avenue Kowloon Tong Hong Kong SAR 999077 China
2
 
Department of Chemistry City University of Hong Kong 83 Tat Chee Avenue Kowloon Hong Kong SAR 999077 China
4
 
Department of Chemistry and Center of Super‐Diamond and Advanced Films (COSDAF) City University of Hong Kong 83 Tat Chee Avenue Hong Kong SAR 999077 China
5
 
Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education and Hubei Key Laboratory of Catalysis and Materials Science South‐Central Minzu University Wuhan 430074 China
6
 
The Shenzhen Research Institute City University of Hong Kong Shenzhen 518057 China
Publication typeJournal Article
Publication date2025-03-20
scimago Q1
wos Q1
SJR9.191
CiteScore43.0
Impact factor27.4
ISSN09359648, 15214095
Abstract

Aqueous zinc ion batteries (AZIBs) face challenges due to the limited interface stability of Zn anode, which includes uncontrolled hydrogen evolution reaction (HER) and excessive dendrite growth. In this study, a natural binary additive composed of saponin and anisaldehyde is introduced to create a stable interfacial adsorption layer for Zn protection via reshaping the electric double layer (EDL) structure. Saponin with rich hydroxyl and carboxyl groups serves as “anchor points”, promoting the adsorption of anisaldehyde through intermolecular hydrogen bonding. Meanwhile, anisaldehyde, with a unique aldehyde group, enhances HER suppression by preferentially facilitating electrocatalytic coupling with H* in the EDL, leading to the formation of a robust inorganic solid electrolyte interphase that prevents dendrite formation, and structural evolution of anisaldehyde during Zn deposition process is verified. As a result, the Zn||Zn symmetric cells present an ultra‐long cycling lifespan of 3 400 h at 1 mA cm−2 and 1 700 h at 10 mA cm−2. Even at the current density of 20 mA cm−2, the cells demonstrate reversible operations for 450 h. Furthermore, Zn‐ion hybrid capacitors exhibit a remarkable lifespan of 100 000 cycles. This work presents a simple synergetic strategy to enhance anode/electrolyte interfacial stability, highlighting its potential for Zn anode protection in high‐performance AZIBs.

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