Hydrated solvation suppression of zinc ions for highly reversible zinc anodes

Jian, Qinping1; Wang, Tianshuai3; Sun, Jing1; Liu, Bin1; Zhao, Tianshou1,2

2023-06-15

10.1016/j.cej.2023.143189

CHEMICAL ENGINEERING JOURNAL   影响因子和分区

1385-8947

1873-3212

Low-cost and high-safety aqueous zinc batteries are promising for large-scale energy storage applications. However, the actual performance of aqueous zinc batteries is hampered by the irreversibility of the zinc metal anode originating from the dendrite growth and side reactions, which are associated closely with the hydrated solvation sheath of Zn2+ ions in aqueous electrolytes. Here, dimethylacetamide is employed as a water dragger agent in low-concentration ZnSO4 electrolytes to reshape the solvation structure of Zn2+ ions. Theoretical cal-culations and experimental investigations reveal that a low fractional addition of dimethylacetamide in aqueous ZnSO4 electrolytes performs strong interactions with water molecules and Zn2+ ions, which inhibits hydrated Zn2+-H2O solvation, facilitates Zn2+-SO42-association and captures free water molecules via H-bonds formation. The coulombic efficiency of Zn plating/stripping is improved from 94.3% to 98.1% and can be stabilized 99.5% over 200 cycles with the hybrid electrolyte. The cycle lifespan of the Zn symmetric cell is prolonged over 1000 h at 1 mA cm-2 and over 450 h at 5 mA cm-2 with the dimethylacetamide-hybrid electrolyte, which are over fourfold higher than that of the pristine ZnSO4 electrolyte. Moreover, when the designed electrolyte incorporated in full cells, the Zn-MnO2 cell exhibits an improved rate performance and an excellent long-term cyclability with a capacity-retention rate of 81% over 2,000 cycles at 1 A g-1. This work provides a feasible strategy for the development of highly stable aqueous zinc batteries.

Zinc anode Electrolyte modulation Solvation regulation Energy storage

SCI ; EI

英语

通讯

Research Grants Council of the Hong Kong Special Administrative Region, China[C5031-20G]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:000994211100001

ELSEVIER SCIENCE SA

20231814043569

Anodes ; Association reactions ; Energy storage ; Hydration ; Ions ; Manganese oxide ; Molecules ; Secondary batteries ; Solvation ; Zinc ; Zinc compounds

Energy Storage:525.7 ; Zinc and Alloys:546.3 ; Electric Batteries and Fuel Cells:702 ; Secondary Batteries:702.1.2 ; Electron Tubes:714.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3

ENGINEERING

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Mech & Aerosp Engn, Clear Water Bay, Hong Kong 999077, Peoples R China
2.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen 518055, Peoples R China
3.Northwestern Polytech Univ, Sch Chem & Chem Engn, Xian 710129, Peoples R China

Jian, Qinping,Wang, Tianshuai,Sun, Jing,et al. Hydrated solvation suppression of zinc ions for highly reversible zinc anodes[J]. CHEMICAL ENGINEERING JOURNAL,2023,466.

Jian, Qinping,Wang, Tianshuai,Sun, Jing,Liu, Bin,&Zhao, Tianshou.(2023).Hydrated solvation suppression of zinc ions for highly reversible zinc anodes.CHEMICAL ENGINEERING JOURNAL,466.

Jian, Qinping,et al."Hydrated solvation suppression of zinc ions for highly reversible zinc anodes".CHEMICAL ENGINEERING JOURNAL 466(2023).