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Vol. 15 (2023)

Effectively Modulating Oxygen Vacancies in Flower-Like δ-MnO2 Nanostructures for Large Capacity and High-Rate Zinc-Ion Storage

https://doi.org/10.1007/s40820-023-01194-3
Yiwei Wang
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Yuxiao Zhang
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Ge Gao
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Yawen Fan
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Ruoxin Wang
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Jie Feng
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Lina Yang
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Alan Meng
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Jian Zhao
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China
Zhenjiang Li
College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, People’s Republic of China

Corresponding Author: Jian Zhao

zjcc2016@qust.edu.cn

Nano-Micro Letters, Vol. 15 (2023), Article Number: 219

Abstract

In recent years, manganese-based oxides as an advanced class of cathode materials for zinc-ion batteries (ZIBs) have attracted a great deal of attentions from numerous researchers. However, their slow reaction kinetics, limited active sites and poor electrical conductivity inevitably give rise to the severe performance degradation. To solve these problems, herein, we introduce abundant oxygen vacancies into the flower-like δ-MnO2 nanostructure and effectively modulate the vacancy defects to reach the optimal level (δ-MnO2−x−2.0). The smart design intrinsically tunes the electronic structure, guarantees ion chemisorption–desorption equilibrium and increases the electroactive sites, which not only effectively accelerates charge transfer rate during reaction processes, but also endows more redox reactions, as verified by first-principle calculations. These merits can help the fabricated δ-MnO2−x−2.0 cathode to present a large specific capacity of 551.8 mAh g−1 at 0.5 A g−1, high-rate capability of 262.2 mAh g−1 at 10 A g−1 and an excellent cycle lifespan (83% of capacity retention after 1500 cycles), which is far superior to those of the other metal compound cathodes. In addition, the charge/discharge mechanism of the δ-MnO2−x−2.0 cathode has also been elaborated through ex situ techniques. This work opens up a new pathway for constructing the next-generation high-performance ZIBs cathode materials.


Highlights:
1 The flower-like δ-MnO2 nanostructures with controlled oxygen vacancies as an extraordinary ZIBs cathode are innovatively developed.
2 The cathode can present large capacity and high-rate zinc-ion storage.
3 DFT analysis substantially unveils the effects of various vacancy concentrations on their electrochemical performances.

Keywords

Znic-ion battery δ-MnO2 cathode materials Oxygen vacancy modulation Large specific capacity High-rate capability
Wang, Yiwei, Yuxiao Zhang, Ge Gao, Yawen Fan, Ruoxin Wang, Jie Feng, Lina Yang, Alan Meng, Jian Zhao, and Zhenjiang Li. 2023. “Effectively Modulating Oxygen Vacancies in Flower-Like δ-MnO2 Nanostructures for Large Capacity and High-Rate Zinc-Ion Storage”. Nano-Micro Letters 15 (October):219. https://doi.org/10.1007/s40820-023-01194-3.
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