Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries

Yueyue He; Sören L. Dreyer; Tolga Akçay; Thomas Diemant; Reiner Mönig; Yuan Ma; Yushu Tang; Huifeng Wang; Jing Lin; Simon Schweidler; Maximilian Fichtner; Horst Hahn; Torsten Brezesinski; Ben Breitung; Yanjiao Ma

doi:10.1021/acsnano.4c07528

Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries

Yueyue He
, Sören L. Dreyer
, Tolga Akçay
, Thomas Diemant
, Reiner Mönig
, Yuan Ma
, Yushu Tang
, Huifeng Wang
, Jing Lin
, Simon Schweidler
, Maximilian Fichtner
, Horst Hahn
, Torsten Brezesinski
, Ben Breitung
, Yanjiao Ma

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Research output: Contribution to journal › Article › peer-review

56 Scopus citations

Abstract

The synergistic engineering of chemical complexity and crystal structures has been applied to Prussian blue analogue (PBA) cathodes in this work. More precisely, the high-entropy concept has been successfully introduced into two structure types of identical composition, namely, cubic and monoclinic. Through the utilization of a variety of complementary characterization techniques, a comprehensive investigation into the electrochemical behavior of the cubic and monoclinic PBAs has been conducted, providing nuanced insights. The implementation of the high-entropy concept exhibits crucial selectivity toward the intrinsic crystal structure. Specifically, while the overall cycling stability of both cathode systems is significantly improved, the synergistic interplay of crystal structure engineering and entropy proves particularly significant. After optimization, the cubic PBA demonstrates structural advantages, showcasing good reversibility, minimal capacity loss, high thermal stability, and unparalleled endurance even under harsh conditions (high specific current and temperature).

Original language	English
Pages (from-to)	24441-24457
Number of pages	17
Journal	ACS Nano
Volume	18
Issue number	35
DOIs	https://doi.org/10.1021/acsnano.4c07528
State	Published - Sep 3 2024

Funding

Y.H. and H.W. acknowledge financial support from the China Scholarship Council (CSC). J.L. acknowledges the Fonds der Chemischen Industrie (FCI) for financial support. The authors further acknowledge the support from the Karlsruhe Nano Micro Facility (KNMFi, www.knmf.kit.edu .), a Helmholtz research infrastructure at Karlsruhe Institute of Technology (KIT, www.kit.edu ). This work contributes to the research performed at CELEST (Center for Electrochemical Energy Storage Ulm-Karlsruhe) and was partly funded by the German Research Foundation (DFG) under project ID 390874152 (POLiS Cluster of Excellence).

Keywords

crystal structure, kinetics
gas evolution
high-entropy materials
phase transition
sodium-ion battery

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10.1021/acsnano.4c07528

Cite this

He, Y., Dreyer, S. L., Akçay, T., Diemant, T., Mönig, R., Ma, Y., Tang, Y., Wang, H., Lin, J., Schweidler, S., Fichtner, M., Hahn, H., Brezesinski, T., Breitung, B., & Ma, Y. (2024). Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries. ACS Nano, 18(35), 24441-24457. https://doi.org/10.1021/acsnano.4c07528

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title = "Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries",

abstract = "The synergistic engineering of chemical complexity and crystal structures has been applied to Prussian blue analogue (PBA) cathodes in this work. More precisely, the high-entropy concept has been successfully introduced into two structure types of identical composition, namely, cubic and monoclinic. Through the utilization of a variety of complementary characterization techniques, a comprehensive investigation into the electrochemical behavior of the cubic and monoclinic PBAs has been conducted, providing nuanced insights. The implementation of the high-entropy concept exhibits crucial selectivity toward the intrinsic crystal structure. Specifically, while the overall cycling stability of both cathode systems is significantly improved, the synergistic interplay of crystal structure engineering and entropy proves particularly significant. After optimization, the cubic PBA demonstrates structural advantages, showcasing good reversibility, minimal capacity loss, high thermal stability, and unparalleled endurance even under harsh conditions (high specific current and temperature).",

keywords = "crystal structure, kinetics, gas evolution, high-entropy materials, phase transition, sodium-ion battery",

author = "Yueyue He and Dreyer, \{S{\"o}ren L.\} and Tolga Ak{\c c}ay and Thomas Diemant and Reiner M{\"o}nig and Yuan Ma and Yushu Tang and Huifeng Wang and Jing Lin and Simon Schweidler and Maximilian Fichtner and Horst Hahn and Torsten Brezesinski and Ben Breitung and Yanjiao Ma",

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He, Y, Dreyer, SL, Akçay, T, Diemant, T, Mönig, R, Ma, Y, Tang, Y, Wang, H, Lin, J, Schweidler, S, Fichtner, M, Hahn, H, Brezesinski, T, Breitung, B & Ma, Y 2024, 'Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries', ACS Nano, vol. 18, no. 35, pp. 24441-24457. https://doi.org/10.1021/acsnano.4c07528

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T1 - Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries

AU - He, Yueyue

AU - Dreyer, Sören L.

AU - Akçay, Tolga

AU - Diemant, Thomas

AU - Mönig, Reiner

AU - Ma, Yuan

AU - Tang, Yushu

AU - Wang, Huifeng

AU - Lin, Jing

AU - Schweidler, Simon

AU - Fichtner, Maximilian

AU - Hahn, Horst

AU - Brezesinski, Torsten

AU - Breitung, Ben

AU - Ma, Yanjiao

PY - 2024/9/3

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N2 - The synergistic engineering of chemical complexity and crystal structures has been applied to Prussian blue analogue (PBA) cathodes in this work. More precisely, the high-entropy concept has been successfully introduced into two structure types of identical composition, namely, cubic and monoclinic. Through the utilization of a variety of complementary characterization techniques, a comprehensive investigation into the electrochemical behavior of the cubic and monoclinic PBAs has been conducted, providing nuanced insights. The implementation of the high-entropy concept exhibits crucial selectivity toward the intrinsic crystal structure. Specifically, while the overall cycling stability of both cathode systems is significantly improved, the synergistic interplay of crystal structure engineering and entropy proves particularly significant. After optimization, the cubic PBA demonstrates structural advantages, showcasing good reversibility, minimal capacity loss, high thermal stability, and unparalleled endurance even under harsh conditions (high specific current and temperature).

AB - The synergistic engineering of chemical complexity and crystal structures has been applied to Prussian blue analogue (PBA) cathodes in this work. More precisely, the high-entropy concept has been successfully introduced into two structure types of identical composition, namely, cubic and monoclinic. Through the utilization of a variety of complementary characterization techniques, a comprehensive investigation into the electrochemical behavior of the cubic and monoclinic PBAs has been conducted, providing nuanced insights. The implementation of the high-entropy concept exhibits crucial selectivity toward the intrinsic crystal structure. Specifically, while the overall cycling stability of both cathode systems is significantly improved, the synergistic interplay of crystal structure engineering and entropy proves particularly significant. After optimization, the cubic PBA demonstrates structural advantages, showcasing good reversibility, minimal capacity loss, high thermal stability, and unparalleled endurance even under harsh conditions (high specific current and temperature).

KW - crystal structure, kinetics

KW - gas evolution

KW - high-entropy materials

KW - phase transition

KW - sodium-ion battery

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Leveraging Entropy and Crystal Structure Engineering in Prussian Blue Analogue Cathodes for Advancing Sodium-Ion Batteries

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