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Recent progress and future prospects of high-entropy materials for battery applications

Wenbo Qiu1, §, Zidong Wang2, §, Shijiang He1, Huaping Zhao2 and Yong Lei2,

+ Author Affiliations

 Corresponding author: Yong Lei, yong.lei@tu-ilmenau.de

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[1]
Qu J, Dai X X, Cui J S, et al. Hierarchical polyaromatic hydrocarbons (PAH) with superior sodium storage properties. J Mater Chem A, 2021, 9, 16554 doi: 10.1039/D1TA03101E
[2]
Yang S Q, Wang P B, Wei H X, et al. Li4V2Mn(PO4)4-stablized Li[Li0.2Mn0.54Ni0.13Co0.13]O2 cathode materials for lithium ion batteries. Nano Energy, 2019, 63, 103889 doi: 10.1016/j.nanoen.2019.103889
[3]
Jiang Z, Li Y H, Han C, et al. Raising lithium storage performances of NaTi2(PO4)3 by nitrogen and sulfur dual-doped carbon layer. J Electrochem Soc, 2020, 167, 020550 doi: 10.1149/1945-7111/ab6c5c
[4]
Chao X, Yan C Z, Zhao H P, et al. Micro-nano structural electrode architecture for high power energy storage. J Semicond, 2023, 44, 050201 doi: 10.1088/1674-4926/44/5/050201
[5]
Wu Y H, Chen G B, Wu X N, et al. Research progress on vanadium oxides for potassium-ion batteries. J Semicond, 2023, 44, 041701 doi: 10.1088/1674-4926/44/4/041701
[6]
Yin Z, Hu M, Liu J, et al. Tunable crystal structure of Cu–Zn–Sn–S nanocrystals for improving photocatalytic hydrogen evolution enabled by copper element regulation. J Semicond, 2022, 43, 032701 doi: 10.1088/1674-4926/43/3/032701
[7]
Li C, Li J, Huang Y B, et al. Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis. J Semicond, 2022, 43, 021701 doi: 10.1088/1674-4926/43/2/021701
[8]
Wang Z D, Hong P, Peng S J, et al. Hierarchitecture Co2(OH)3 Cl@FeCo2O4 composite as a novel and high-performance electrode material applied in supercapacitor. Int J Energy Res, 2020, 44, 3122 doi: 10.1002/er.5152
[9]
Wang Z D, Hong P, Zhao H P, et al. Recent developments and future prospects of transition metal compounds as electrode materials for potassium-ion hybrid capacitors. Adv Mater Technol, 2023, 8, 2200515 doi: 10.1002/admt.202200515
[10]
Qu J, Sheng T, Wu Z G, et al. Unexpected effects of zirconium-doping in the high performance sodium manganese-based layer-tunnel cathode. J Mater Chem A, 2018, 6, 13934 doi: 10.1039/C8TA04818E
[11]
He S J, Wang Z D, Wang Z J, et al. Recent progress and future prospect of novel multi-ion storage devices. J Semicond, 2023, 44, 040201 doi: 10.1088/1674-4926/44/4/040201
[12]
Zhang Y Q, Wang D D, Wang S Y. High-entropy alloys for electrocatalysis: Design, characterization, and applications. Small, 2022, 18, e2104339 doi: 10.1002/smll.202104339
[13]
Sarkar A, Wang Q S, Schiele A, et al. High-entropy oxides: Fundamental aspects and electrochemical properties. Adv Mater, 2019, 31, e1806236 doi: 10.1002/adma.201806236
[14]
Sarkar A, Velasco L, Wang D, et al. High entropy oxides for reversible energy storage. Nat Commun, 2018, 9, 3400 doi: 10.1038/s41467-018-05774-5
[15]
Stygar M, Dąbrowa J, Moździerz M, et al. Formation and properties of high entropy oxides in Co-Cr-Fe-Mg-Mn-Ni-O system: Novel (Cr, Fe, Mg, Mn, Ni)3O4 and (Co, Cr, Fe, Mg, Mn)3O4 high entropy spinels. J Eur Ceram Soc, 2020, 40, 1644 doi: 10.1016/j.jeurceramsoc.2019.11.030
[16]
Rost C M, Sachet E, Borman T, et al. Entropy-stabilized oxides. Nat Commun, 2015, 6, 8485 doi: 10.1038/ncomms9485
[17]
Sukkurji P A, Cui Y Y, Lee S, et al. Mechanochemical synthesis of novel rutile-type high entropy fluorides for electrocatalysis. J Mater Chem A, 2021, 9, 8998 doi: 10.1039/D0TA10209A
[18]
Nguyen T X, Su Y H, Lin C C, et al. Self-reconstruction of sulfate-containing high entropy sulfide for exceptionally high-performance oxygen evolution reaction electrocatalyst. Adv Funct Materials, 2021, 31(48), 2106229 doi: 10.1002/adfm.202106229
[19]
Gao M C, Miracle D B, Maurice D, et al. High-entropy functional materials. J Mater Res, 2018, 33, 3138 doi: 10.1557/jmr.2018.323
[20]
Senkov O N. A critical review of high entropy alloys and related concepts. Acta Mater, 2017, 122, 448 doi: 10.1016/j.actamat.2016.08.081
[21]
Zhou P F, Che Z N, Liu J, et al. High-entropy P2/O3 biphasic cathode materials for wide-temperature rechargeable sodium-ion batteries. Energy Storage Mater, 2023, 57, 618 doi: 10.1016/j.ensm.2023.03.007
[22]
Joshi A, Chakrabarty S, Akella S H, et al. High-entropy co-free O3- type layered oxyfluoride: A promising air-stable cathode for sodium-ion batteries. Adv Mater, 2023, 35, e2304440 doi: 10.1002/adma.202304440
[23]
Huang Y, Zhang X, Ji L, et al. Boosting the sodium storage performance of Prussian blue analogs by single-crystal and high-entropy approach. Energy Storage Mater, 2023, 58, 1 doi: 10.1016/j.ensm.2023.03.011
[24]
Zhao X, Xing Z H, Huang C D. Investigation of high-entropy Prussian blue analog as cathode material for aqueous sodium-ion batteries. J Mater Chem A, 2023, 11, 22835 doi: 10.1039/D3TA04349E
[25]
Gu Z Y, Guo J Z, Cao J M, et al. An advanced high-entropy fluorophosphate cathode for sodium-ion batteries with increased working voltage and energy density. Adv Mater, 2022, 34, e2110108 doi: 10.1002/adma.202110108
[26]
Liu C, Bi J Q, Xie L L, et al. High entropy spinel oxides (CrFeMnNiCo x )3O4 (x = 2, 3, 4) nanoparticles as anode material towards electrochemical properties. J Energy Storage, 2023, 71, 108211 doi: 10.1016/j.est.2023.108211
[27]
Yang X B, Wang H Q, Song Y Y, et al. Low-temperature synthesis of a porous high-entropy transition-metal oxide as an anode for high-performance lithium-ion batteries. ACS Appl Mater Interfaces, 2022, 14(23), 26873 doi: 10.1021/acsami.2c07576
[28]
Brandt T G, Tuokkola A R, Yu M J, et al. Liquid-feed flame spray pyrolysis enabled synthesis of Co- and Cr-free, high-entropy spinel oxides as Li-ion anodes. Chem Eng J, 2023, 474, 145495 doi: 10.1016/j.cej.2023.145495
[29]
Lin L, Wang K, Sarkar A, et al. High-entropy sulfides as electrode materials for Li-ion batteries. Adv Energy Mater, 2022, 12, 2103090 doi: 10.1002/aenm.202103090
[30]
Zhao J, Zhang Y, Chen X, et al. Entropy-change driven highly reversible sodium storage for conversion-type sulfide. Adv Funct Materials, 2022, 32, 2206531 doi: 10.1002/adfm.202206531
Fig. 1.  (Color online) (a) P2/O3 biphasic cathodes’ P2/O3 ratios at different temperatures, (b) initial charge/discharge curves, and (c) cycling performance over a wide operating temperature range (−40 to 50 ℃), respectively. Reproduced with permission[21], Copyright 2023, Elsevier. (d) Cycling performance (at 100 mA·g−1), (e) rate performance of PC-HEPBA, SC-HEPBA and Mixture. Reproduced with permission[23], Copyright 2023, Elsevier. (f) Schematic drawing for crystal structure change from p-NVPF to HE-NVPF. (g) GCD curves of HE-NVPF cathode, and (h) the calculated capacity contribution of the discharge voltage interval (2.0−3.4 V). Reproduced with permission[25], Copyright 2023, Wiley.

Fig. 2.  (Color online) (a) Schematic drawing of ion transmission path within the conventional material and the new-type HEMs. (b) Long cycling performance and (c) rate performance of HEO-450, HEO-850, and FEO, respectively. Reproduced with permission[27], Copyright 2023, American Chemical Society. (d) Contribution of synthetic metals to HEO price, (e) synthesized HEO anodes’ cost-effectiveness. Reproduced with permission[28], Copyright 2022, Elsevier. (f) At different current densities and in the voltage range between 0.01 and 3 V, Li+/Li rate performance of all HESs, CoS2, 4MS2, and MWCNTs half-cell[29], Copyright 2022, Wiley. Comparison with ex-situ XRD patterns for the (g) Cu2MnSnS4 (CSS) and (j) HE-CMFSGS discharged after different cycle numbers (1st, 10th, and 20th). And (h, i, k, l) TEM images from the diffraction of the Sn (200) plane. Reproduced with permission[30], Copyright 2022, Wiley.

[1]
Qu J, Dai X X, Cui J S, et al. Hierarchical polyaromatic hydrocarbons (PAH) with superior sodium storage properties. J Mater Chem A, 2021, 9, 16554 doi: 10.1039/D1TA03101E
[2]
Yang S Q, Wang P B, Wei H X, et al. Li4V2Mn(PO4)4-stablized Li[Li0.2Mn0.54Ni0.13Co0.13]O2 cathode materials for lithium ion batteries. Nano Energy, 2019, 63, 103889 doi: 10.1016/j.nanoen.2019.103889
[3]
Jiang Z, Li Y H, Han C, et al. Raising lithium storage performances of NaTi2(PO4)3 by nitrogen and sulfur dual-doped carbon layer. J Electrochem Soc, 2020, 167, 020550 doi: 10.1149/1945-7111/ab6c5c
[4]
Chao X, Yan C Z, Zhao H P, et al. Micro-nano structural electrode architecture for high power energy storage. J Semicond, 2023, 44, 050201 doi: 10.1088/1674-4926/44/5/050201
[5]
Wu Y H, Chen G B, Wu X N, et al. Research progress on vanadium oxides for potassium-ion batteries. J Semicond, 2023, 44, 041701 doi: 10.1088/1674-4926/44/4/041701
[6]
Yin Z, Hu M, Liu J, et al. Tunable crystal structure of Cu–Zn–Sn–S nanocrystals for improving photocatalytic hydrogen evolution enabled by copper element regulation. J Semicond, 2022, 43, 032701 doi: 10.1088/1674-4926/43/3/032701
[7]
Li C, Li J, Huang Y B, et al. Recent development in electronic structure tuning of graphitic carbon nitride for highly efficient photocatalysis. J Semicond, 2022, 43, 021701 doi: 10.1088/1674-4926/43/2/021701
[8]
Wang Z D, Hong P, Peng S J, et al. Hierarchitecture Co2(OH)3 Cl@FeCo2O4 composite as a novel and high-performance electrode material applied in supercapacitor. Int J Energy Res, 2020, 44, 3122 doi: 10.1002/er.5152
[9]
Wang Z D, Hong P, Zhao H P, et al. Recent developments and future prospects of transition metal compounds as electrode materials for potassium-ion hybrid capacitors. Adv Mater Technol, 2023, 8, 2200515 doi: 10.1002/admt.202200515
[10]
Qu J, Sheng T, Wu Z G, et al. Unexpected effects of zirconium-doping in the high performance sodium manganese-based layer-tunnel cathode. J Mater Chem A, 2018, 6, 13934 doi: 10.1039/C8TA04818E
[11]
He S J, Wang Z D, Wang Z J, et al. Recent progress and future prospect of novel multi-ion storage devices. J Semicond, 2023, 44, 040201 doi: 10.1088/1674-4926/44/4/040201
[12]
Zhang Y Q, Wang D D, Wang S Y. High-entropy alloys for electrocatalysis: Design, characterization, and applications. Small, 2022, 18, e2104339 doi: 10.1002/smll.202104339
[13]
Sarkar A, Wang Q S, Schiele A, et al. High-entropy oxides: Fundamental aspects and electrochemical properties. Adv Mater, 2019, 31, e1806236 doi: 10.1002/adma.201806236
[14]
Sarkar A, Velasco L, Wang D, et al. High entropy oxides for reversible energy storage. Nat Commun, 2018, 9, 3400 doi: 10.1038/s41467-018-05774-5
[15]
Stygar M, Dąbrowa J, Moździerz M, et al. Formation and properties of high entropy oxides in Co-Cr-Fe-Mg-Mn-Ni-O system: Novel (Cr, Fe, Mg, Mn, Ni)3O4 and (Co, Cr, Fe, Mg, Mn)3O4 high entropy spinels. J Eur Ceram Soc, 2020, 40, 1644 doi: 10.1016/j.jeurceramsoc.2019.11.030
[16]
Rost C M, Sachet E, Borman T, et al. Entropy-stabilized oxides. Nat Commun, 2015, 6, 8485 doi: 10.1038/ncomms9485
[17]
Sukkurji P A, Cui Y Y, Lee S, et al. Mechanochemical synthesis of novel rutile-type high entropy fluorides for electrocatalysis. J Mater Chem A, 2021, 9, 8998 doi: 10.1039/D0TA10209A
[18]
Nguyen T X, Su Y H, Lin C C, et al. Self-reconstruction of sulfate-containing high entropy sulfide for exceptionally high-performance oxygen evolution reaction electrocatalyst. Adv Funct Materials, 2021, 31(48), 2106229 doi: 10.1002/adfm.202106229
[19]
Gao M C, Miracle D B, Maurice D, et al. High-entropy functional materials. J Mater Res, 2018, 33, 3138 doi: 10.1557/jmr.2018.323
[20]
Senkov O N. A critical review of high entropy alloys and related concepts. Acta Mater, 2017, 122, 448 doi: 10.1016/j.actamat.2016.08.081
[21]
Zhou P F, Che Z N, Liu J, et al. High-entropy P2/O3 biphasic cathode materials for wide-temperature rechargeable sodium-ion batteries. Energy Storage Mater, 2023, 57, 618 doi: 10.1016/j.ensm.2023.03.007
[22]
Joshi A, Chakrabarty S, Akella S H, et al. High-entropy co-free O3- type layered oxyfluoride: A promising air-stable cathode for sodium-ion batteries. Adv Mater, 2023, 35, e2304440 doi: 10.1002/adma.202304440
[23]
Huang Y, Zhang X, Ji L, et al. Boosting the sodium storage performance of Prussian blue analogs by single-crystal and high-entropy approach. Energy Storage Mater, 2023, 58, 1 doi: 10.1016/j.ensm.2023.03.011
[24]
Zhao X, Xing Z H, Huang C D. Investigation of high-entropy Prussian blue analog as cathode material for aqueous sodium-ion batteries. J Mater Chem A, 2023, 11, 22835 doi: 10.1039/D3TA04349E
[25]
Gu Z Y, Guo J Z, Cao J M, et al. An advanced high-entropy fluorophosphate cathode for sodium-ion batteries with increased working voltage and energy density. Adv Mater, 2022, 34, e2110108 doi: 10.1002/adma.202110108
[26]
Liu C, Bi J Q, Xie L L, et al. High entropy spinel oxides (CrFeMnNiCo x )3O4 (x = 2, 3, 4) nanoparticles as anode material towards electrochemical properties. J Energy Storage, 2023, 71, 108211 doi: 10.1016/j.est.2023.108211
[27]
Yang X B, Wang H Q, Song Y Y, et al. Low-temperature synthesis of a porous high-entropy transition-metal oxide as an anode for high-performance lithium-ion batteries. ACS Appl Mater Interfaces, 2022, 14(23), 26873 doi: 10.1021/acsami.2c07576
[28]
Brandt T G, Tuokkola A R, Yu M J, et al. Liquid-feed flame spray pyrolysis enabled synthesis of Co- and Cr-free, high-entropy spinel oxides as Li-ion anodes. Chem Eng J, 2023, 474, 145495 doi: 10.1016/j.cej.2023.145495
[29]
Lin L, Wang K, Sarkar A, et al. High-entropy sulfides as electrode materials for Li-ion batteries. Adv Energy Mater, 2022, 12, 2103090 doi: 10.1002/aenm.202103090
[30]
Zhao J, Zhang Y, Chen X, et al. Entropy-change driven highly reversible sodium storage for conversion-type sulfide. Adv Funct Materials, 2022, 32, 2206531 doi: 10.1002/adfm.202206531
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    Received: 01 January 2024 Revised: 20 January 2024 Online: Accepted Manuscript: 29 January 2024Uncorrected proof: 30 January 2024Published: 15 March 2024

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      Wenbo Qiu, Zidong Wang, Shijiang He, Huaping Zhao, Yong Lei. Recent progress and future prospects of high-entropy materials for battery applications[J]. Journal of Semiconductors, 2024, 45(3): 030202. doi: 10.1088/1674-4926/45/3/030202 W B Qiu, Z D Wang, S J He, H P Zhao, Y Lei. Recent progress and future prospects of high-entropy materials for battery applications[J]. J. Semicond, 2024, 45(3): 030202. doi: 10.1088/1674-4926/45/3/030202Export: BibTex EndNote
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      Wenbo Qiu, Zidong Wang, Shijiang He, Huaping Zhao, Yong Lei. Recent progress and future prospects of high-entropy materials for battery applications[J]. Journal of Semiconductors, 2024, 45(3): 030202. doi: 10.1088/1674-4926/45/3/030202

      W B Qiu, Z D Wang, S J He, H P Zhao, Y Lei. Recent progress and future prospects of high-entropy materials for battery applications[J]. J. Semicond, 2024, 45(3): 030202. doi: 10.1088/1674-4926/45/3/030202
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      Recent progress and future prospects of high-entropy materials for battery applications

      doi: 10.1088/1674-4926/45/3/030202
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      • Author Bio:

        Wenbo Qiu Wenbo Qiu got her BS degree from Jiujiang University in 2022. Currently, she is pursuing her Master’s Degree at Shanghai University. Her research interests focus on the construction and functionalization of nanomaterials for energy storage devices

        Zidong Wang Zidong Wang received his M.S. degree in materials physics and chemistry from Yunnan University in 2020. He is currently a Ph.D. student under the supervision of Prof. Yong Lei at the Technical University of Ilmenau in Germany. His research interests focus on designing and synthesizing nanostructural inorganic materials for electrochemical energy storage

        Shijiang He Shijiang He got his BS degree from Changzhou University in 2021. Now he is a M.S. student at the Shanghai University. His research interests focus on the construction and functionalization of nanomaterials for energy storage devices

        Huaping Zhao Huaping Zhao obtained his PhD from Shandong University in 2007. Following two years postdoc research at the Institute of Chemistry (Chinese Academy of Sciences, 2007–2009), he worked as a scientist by the University of Muenster from 2009 to 2011. Since 2012, he has been a senior scientist in Prof. Yong Lei’s group at the Technical University of Ilmenau, Germany. His current research focus is the design and fabrication of functional nanostructures for energy storage and conversion

        Yong Lei Yong Lei is Professor and the Head of Department (Chair) of Applied Nano-Physics at the Technical University of Ilmenau, Germany. He started to work in Germany as an Alexander von Humboldt Fellow at Karlsruhe Institute of Technology in 2003. From 2006 he worked at University of Muenster as a group leader and Junior Professor. In 2011 he joined the Technical University of Ilmenau as a Professor. His research focuses include template nanostructuring, energy conversion and storage devices, and optoelectronic applications of functional nanostructures. He received a few prestigious funding in Europe and Germany such as two European Research Council Grants. Prof. Lei is Advisory Board Member or Associate Editor of a few journals such as Advanced Energy Materials, Energy & Environmental Materials, InfoMat, Carbon Energy, Science China Materials and Journal of Semiconductors

      • Corresponding author: yong.lei@tu-ilmenau.de
      • Received Date: 2024-01-01
      • Revised Date: 2024-01-20
      • Available Online: 2024-01-29

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