Manipulating Interfacial Stability Via Absorption-Competition Mechanism for Long-Lifespan Zn Anode

Meijia Qiu; Liang Ma; Peng Sun; Zilong Wang; Guofeng Cui; Wenjie Mai

doi:10.1007/s40820-021-00777-2

Manipulating Interfacial Stability Via Absorption-Competition Mechanism for Long-Lifespan Zn Anode

Nanomicro Lett. 2021 Dec 13;14(1):31. doi: 10.1007/s40820-021-00777-2.

Authors

Meijia Qiu^{1

2}, Liang Ma², Peng Sun^{1

2}, Zilong Wang², Guofeng Cui³, Wenjie Mai²

Affiliations

¹ Key Laboratory for Polymeric Composite & Functional Materials of Ministry of Education, School of Chemistry, Key Laboratory of Low-Carbon Chemistry & Energy Conservation of Guangdong Province, Sun Yat-Sen University, Guangzhou, 510275, People's Republic of China.
² Siyuan Laboratory, Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University, Guangdong, 510632, People's Republic of China.
³ Key Laboratory for Polymeric Composite & Functional Materials of Ministry of Education, School of Chemistry, Key Laboratory of Low-Carbon Chemistry & Energy Conservation of Guangdong Province, Sun Yat-Sen University, Guangzhou, 510275, People's Republic of China. cuigf@mail.sysu.edu.cn.

Abstract

The stability of Zn anode in various Zn-based energy storage devices is the key problem to be solved. Herein, aromatic aldehyde additives are selected to modulate the interface reactions between the Zn anode and electrolyte. Through comprehensively considering electrochemical measurements, DFT calculations and FEA simulations, novel mechanisms of one kind of aromatic aldehyde, veratraldehyde in inhibiting Zn dendrite/by-products can be obtained. This additive prefers to absorb on the Zn surface than H₂O molecules and Zn²⁺, while competes with hydrogen evolution reaction and Zn plating/stripping process via redox reactions, thus preventing the decomposition of active H₂O near the interface and uncontrollable Zn dendrite growth via a synactic absorption-competition mechanism. As a result, Zn-Zn symmetric cells with the veratraldehyde additive realize an excellent cycling life of 3200 h under 1 mA cm^-2/1 mAh cm^-2 and over 800 h even under 5 mA cm^-2/5 mAh cm^-2. Moreover, Zn-Ti and Zn-MnO₂ cells with the veratraldehyde additive both obtain elevated performance than that with pure ZnSO₄ electrolyte. Finally, two more aromatic aldehyde additives are chosen to prove their universality in stabilizing Zn anodes.

Keywords: Absorption-competition mechanism; Aromatic aldehyde; Interfacial stability; Zn anode.