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Title: High-Voltage Potassium Hexacyanoferrate Cathode via High-Entropy and Potassium Incorporation for Stable Sodium-Ion Batteries

Journal Article · · ACS Nano

Prussian blue analogues (PBAs) used as sodium ion battery (SIB) cathodes are usually the focus of attention due to their three-dimensional open frame and high theoretical capacity. Nonetheless, the disadvantages of a low working voltage and inferior structural stability of PBAs prevent their further applications. Herein, we propose constructing the Kx(MnFeCoNiCu)[Fe(CN)6] (HE-K-PBA) cathode by high-entropy and potassium incorporation strategy to simultaneously realize high working voltage and cycling stability. In this study, the reaction mechanism of metal cations in HE-K-PBA are revealed by synchrotron radiation X-ray absorption spectroscopy (XAS), ex situ X-ray photoelectron spectroscopy (XPS), and in situ Raman spectra. We also investigate the entropy stabilization mechanism via finite element simulation, demonstrating that HE-K-PBA with small von Mises stress and weak structure strain can significantly mitigate the structural distortion. Benefit from the stable structure and everlasting K+ (de)intercalation, the HE-K-PBA delivers high output voltage (3.46 V), good reversible capacity (120.5 mAh g–1 at 0.01 A g–1), and capacity retention of 90.4% after 1700 cycles at 1.0 A g–1. Moreover, the assembled full cell and all-solid-state batteries with a stable median voltage of 3.29 V over 3000 cycles further demonstrate the application prospects of the HE-K-PBA cathode.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704
OSTI ID:
2205648
Report Number(s):
BNL--224995-2023-JAAM; {"","Journal ID: ISSN 1936-0851"}
Journal Information:
ACS Nano, Journal Name: ACS Nano Journal Issue: 21 Vol. 17; ISSN 1936-0851
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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