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@ARTICLE{He:1025145,
author = {He, Yueyue and Dreyer, Sören L. and Ting, Yin-Ying and Ma,
Yuan and Hu, Yang and Goonetilleke, Damian and Tang, Yushu
and Diemant, Thomas and Zhou, Bei and Kowalski, Piotr M. and
Fichtner, Maximilian and Hahn, Horst and Aghassi-Hagmann,
Jasmin and Brezesinski, Torsten and Breitung, Ben and Ma,
Yanjiao},
title = {{E}ntropy‐{M}ediated {S}table {S}tructural {E}volution of
{P}russian {W}hite {C}athodes for {L}ong‐{L}ife
{N}a‐{I}on {B}atteries},
journal = {Angewandte Chemie},
volume = {136},
number = {7},
issn = {0932-2132},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2024-02722},
pages = {e202315371},
year = {2024},
abstract = {The high-entropy approach is applied to monoclinic Prussian
White (PW) Na-ion cathodes to address the issue of
unfavorable multilevel phase transitions upon
electrochemical cycling, leading to poor stability and
capacity decay. A series of Mn-based samples with up to six
metal species sharing the N-coordinated positions was
synthesized. The material of composition
Na1.65Mn0.4Fe0.12Ni0.12Cu0.12Co0.12Cd0.12[Fe(CN)6]0.92□0.08 ⋅ 1.09H2O
was found to exhibit superior cyclability over
medium/low-entropy and conventional single-metal PWs. We
also report, to our knowledge for the first time, that a
high-symmetry crystal structure may be advantageous for
high-entropy PWs during battery operation. Computational
comparisons of the formation enthalpy demonstrate that the
compositionally less complex materials are prone to phase
transitions, which negatively affect cycling performance.
Based on data from complementary characterization
techniques, an intrinsic mechanism for the stability
improvement of the disordered PW structure upon Na+
insertion/extraction is proposed, namely the dual effect of
suppression of phase transitions and mitigation of gas
evolution.},
cin = {IEK-13},
ddc = {660},
cid = {I:(DE-Juel1)IEK-13-20190226},
pnm = {1212 - Materials and Interfaces (POF4-121)},
pid = {G:(DE-HGF)POF4-1212},
typ = {PUB:(DE-HGF)16},
doi = {10.1002/ange.202315371},
url = {https://juser.fz-juelich.de/record/1025145},
}