J. Semicond. > 2024, Volume 45 > Issue 2 > 021801, doi: 10.1088/1674-4926/45/2/021801
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REVIEWS

Research progress of alkaline earth metal iron-based oxides as anodes for lithium-ion batteries

Mingyuan Ye1, §, Xiaorui Hao2, §, Jinfeng Zeng3, Lin Li4, , Pengfei Wang1, Chenglin Zhang5, , Li Liu1, Fanian Shi1, and Yuhan Wu1, 6,

+ Author Affiliations

 Corresponding author: Lin Li, linli@wzu.edu.cn; Chenglin Zhang, chenglinzhang@ujs.edu.cn; Fanian Shi, shifn@sut.edu.cn; Yuhan Wu, yuhanwu@sut.edu.cn

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Abstract: Anode materials are an essential part of lithium-ion batteries (LIBs), which determine the performance and safety of LIBs. Currently, graphite, as the anode material of commercial LIBs, is limited by its low theoretical capacity of 372 mA·h·g−1, thus hindering further development toward high-capacity and large-scale applications. Alkaline earth metal iron-based oxides are considered a promising candidate to replace graphite because of their low preparation cost, good thermal stability, superior stability, and high electrochemical performance. Nonetheless, many issues and challenges remain to be addressed. Herein, we systematically summarize the research progress of alkaline earth metal iron-based oxides as LIB anodes. Meanwhile, the material and structural properties, synthesis methods, electrochemical reaction mechanisms, and improvement strategies are introduced. Finally, existing challenges and future research directions are discussed to accelerate their practical application in commercial LIBs.

Key words: alkali-earth metal iron-based oxides, anodes, lithium-ion batteries, electrochemical energy storage



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Fig. 1.  (Color online) The classification of alkaline earth metal iron oxides and their representative materials as anodes for LIBs.

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Fig. 2.  (Color online) Representative structure of spinel ferrite oxides viewed down the (001) axis. Cations occupy tetrahedral (8a) sites and octahedral (16d) sites, with oxygen atoms at the 32e sites. Octahedral (16c) vacancies in the structure are also indicated[30]. (Reprinted with permission, Copyright 2020, The Royal Society of Chemistry).

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Fig. 3.  (Color online) Transmission electron microscope (TEM) images of MgFe2O4 spinel: (a) as-prepared and (b) 15 h milled. (c) Cyclic performance of MgFe2O4 spinel samples: (A) as-prepared and (B) 15 h milled sample[36] (Reprinted with permission, Copyright 2011, Elsevier). (d) SEM images of MgFe2O4 microboxes. (e) Cyclic voltammetry curves of the MOF MgFe2O4 sample at a scan rate of 0.1 mV·s−1. (f) Rate performance of the MgFe2O4 derived from MOF and sol-gel methods at current densities from 0.05 to 1.0 A·g−1. (g) Charge/discharge curves of the MgFe2O4 derived from MOF and sol-gel methods at a current density of 50 mA·g−1. (h) Cyclic performance of MOF MgFe2O4 for the first 550 cycles at a current density of 1.0 and 5.0 A·g−1[45] (Reprinted with permission, Copyright 2017, Elsevier).

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Fig. 4.  (Color online) (a) Schematic representation of the synthetic process of MgFe2O4/G. (b) The cycle performance of MgFe2O4/G and MgFe2O4 at 500 mA·g−1[61] (Reprinted with permission, Copyright 2017, The American Chemical Society). (c) MgFe2O4/C rate capacity and Coulombic efficiency at 200−3000 mA·g−1. (d) Schematic representation of the lithium insertion/de-insertion in the MgFe2O4 structure[62] (Reprinted with permission, Copyright 2020, Elsevier). (e) Synthetic plot and (f) FESEM plot of the MFO/NPCNF. The cycle performance of NPCNF and MFO/NPCNF at (g) 0.5 A·g−1 and (h) 1 A·g−1[64] (Reprinted with permission, Copyright 2021, Elsevier). (i) Schematic diagram of the structure design for the PAN-MgFe2O4 flexible free-standing anode. (j) Modeling and optimized structure of MgFe2O4/Fe3N heterojunction. (k) Electronic density of states of MgFe2O4/Fe3N heterojunction. (l) MgFe2O4/Fe3N heterojunction differential charge density (isosurface level: 0.015). (m) Adsorption structure of lithium-ions at the MgFe2O4/Fe3N heterogeneous interface[72] (Reprinted with permission, Copyright 2022, The American Chemical Society).

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Fig. 5.  (Color online) (a) Schematic illustration of the synthesis of CaFe2O4 via solution combustion technique. (b) HR-FESEM images of as-synthesized CaFe2O4. (c) Schematic illustration of lithium insertion into CaFe2O4 anode. (d) Cycling performance at a current density of 500 mA·g−1 up to 500 cycles[84] (Reprinted with permission, Copyright 2019, Elsevier). (e) TEM image of sintered CaFe2O4 nanofibers. (f) Crystal structure of CaFe2O4 nanofibers[85] (Reprinted with permission, Copyright 2020, IOPscience).

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Fig. 6.  (Color online) Unit cell diagram of SrFe12O19. Two large green spheres represent Sr atoms, while small red spheres represent O atoms. Fe atoms in each site are presented in different colors: 2a (blue), 4f1 (gray), 12k (pink), 4f2 (yellow), and 2b (purple)[91] (Reprinted with permission, Copyright 2021, Elsevier).

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Fig. 7.  (Color online) (a) XRD patterns of SrFe12O19 at different annealing temperatures. (b) FESEM image of SrFe12O19[93] (Reprinted with permission, Copyright 2018, Elsevier). (c) TEM images of the as-prepared BaFe12O19. (d) Cycle performance of BaFe12O19 electrode[94] (Reprinted with permission, Copyright 2013, Springer). (e) Cycling performance of BaFe12O19 and Zn2+-doped BaFe12O19 nanoplates at a current density of 100 mA·g−1 and columbic efficiency of Zn2+-doped BaFe12O19 nanoplates[95] (Reprinted with permission, Copyright 2015, The Royal Society of Chemistry). (f) XRD pattern of the powders synthesized by different Fe/Sr ratios. (g) SEM images of Zn2+-doped SrFe12O19 nanoplates[96] (Reprinted with permission, Copyright 2017, The Royal Society of Chemistry).

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Fig. 8.  (Color online) Design principles for realizing polar structures from nonpolar compounds through anion-vacancy and cation order. Starting from (a) fully oxidized perovskites are reduced in Step 1, resulting in (b) ordered rows of oxygen vacancies forming alternating layers of BO6 octahedra and BO4 tetrahedra. (c−e) Depict the resulting ABO2.5 brownmillerites: the polar I2 cm and the nonpolar Pbcm and Pnam polymorphs that arise owing to the relative alignment of the BO4 tetrahedra. Inversion centers are located at sites with octahedrally coordinated B cations, indicated by black open circles; not shown are the inversion centers situated on the unoccupied sites in the Pbcm and Pnam polymorphs. (f) In Step 2, chemically distinct A and A′ cations are ordered in layers along the ···BO6–BO4–BO6··· chain direction, which then removes all inversion centers and permits the net electric polarizations P indicated in (g)[97] (Reprinted with permission, Copyright 2017, The American Chemical Society).

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Fig. 9.  (Color online) (a) Schematic illustration of lithium insertion/de-insertion in Ca2Fe2O5 nanoparticles and nanofibers. (b) XPS and (c) EPR of nanofibers of Ca2Fe2O5[98] (Reprinted with permission, Copyright 2020, The American Chemical Society). (d) Rate performance of C2FONF-900. (e) Comparative cyclic performance in Ca2Fe2O5 electrodes in different annealing temperatures. (f) CV curves of C2FONF-900 at various scan rates. (g) log i vs. log v plot of C2FONF-900[103]. Copyright 2021, Elsevier.

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Fig. 10.  (Color online) Possible future development directions of alkaline earth metal iron-based oxide anodes.

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Table 1.   Comparing the physical, chemical, and economic parameters of alkaline earth metal elements.

MgCaSrBa
Atomic number12203856
Atomic mass (g·mol−1)24.30540.07887.62137.327
Abundance in earth's crust (%)2.334.150.0370.0425
Melting point (°C)651842769725
Ionic radius (Å)0.7211.181.35
Distribution22.5% in ChinaEverywhere37.9% in Spain29% in China
Price of nitrate
(US $ per kg)		2.232.216.530.246
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Table 2.   Comparison of the cycling performance of alkaline earth metal MFe2O4-based electrodes.

Materials (morphological structure) Synthesis methods Reversible capacity (mA·h·g−1)/Cycle times Current density (mA·g−1) Refs
MgFe2O4 nanomicrospheres Solvothermal method 634/350th 500 [73]
Submicron hollow spherical MgFe2O4 Solvothermal method 900/70th 107.2 [74]
Porous CaFe2O4 Sol-gel method 816/100th 100 [75]
Carbon-coated MgFe2O4 Coprecipitation method 744/160th 100 [76]
Nitrogen-doped carbon-coated MgFe2O4 nanofibers Electrospinning method 926/200th 100 [77]
Coralline Fe2O3@MgFe2O4 Gel-cast method 1700/500th 100 [78]
Double-shelled hybrid MgFe2O4@Fe2O3 hollow microspheres Hydrothermal method 1390/160th 500 [79]
3D porous MgFe2O4 Hydrothermal method 780/1000th 5000 [80]
MgFe2O4@ZnFe2O4@MgO irregular nanosheets Thermal decomposition and selective etching 500/330th 100 [81]
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    Received: 20 September 2023 Revised: 18 October 2023 Online: Accepted Manuscript: 13 November 2023Uncorrected proof: 08 December 2023Published: 10 February 2024

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      Article Navigation >  Journal of Semiconductors  > 2024  >  45(2): 021801
      Mingyuan Ye, Xiaorui Hao, Jinfeng Zeng, Lin Li, Pengfei Wang, Chenglin Zhang, Li Liu, Fanian Shi, Yuhan Wu. Research progress of alkaline earth metal iron-based oxides as anodes for lithium-ion batteries[J]. Journal of Semiconductors, 2024, 45(2): 021801. doi: 10.1088/1674-4926/45/2/021801 M Y Ye, X R Hao, J F Zeng, L Li, P F Wang, C L Zhang, L Liu, F N Shi, Y H Wu. Research progress of alkaline earth metal iron-based oxides as anodes for lithium-ion batteries[J]. J. Semicond, 2024, 45(2): 021801. doi: 10.1088/1674-4926/45/2/021801Export: BibTex EndNote
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      Mingyuan Ye, Xiaorui Hao, Jinfeng Zeng, Lin Li, Pengfei Wang, Chenglin Zhang, Li Liu, Fanian Shi, Yuhan Wu. Research progress of alkaline earth metal iron-based oxides as anodes for lithium-ion batteries[J]. Journal of Semiconductors, 2024, 45(2): 021801. doi: 10.1088/1674-4926/45/2/021801

      M Y Ye, X R Hao, J F Zeng, L Li, P F Wang, C L Zhang, L Liu, F N Shi, Y H Wu. Research progress of alkaline earth metal iron-based oxides as anodes for lithium-ion batteries[J]. J. Semicond, 2024, 45(2): 021801. doi: 10.1088/1674-4926/45/2/021801
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      Research progress of alkaline earth metal iron-based oxides as anodes for lithium-ion batteries

      doi: 10.1088/1674-4926/45/2/021801
      • 1.

        School of Environmental and Chemical Engineering, Shenyang University of Technology, Shenyang 110870, China

      • 2.

        College of Materials Science and Engineering, Nanjing Tech University, Nanjing 211816, China

      • 3.

        College of Pharmacy, Xinjiang Medical University, Engineering Research Center of Xinjiang and Central Asian Medicine Resources (Ministry of Education), Urumqi 830000, China

      • 4.

        Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, China

      • 5.

        School of Physics and Electronic Engineering, Jiangsu University, Zhenjiang 212013, China

      • 6.

        Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin 300071, China

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      • Author Bio:

        Mingyuan Ye Mingyuan Ye is currently a graduate student at Shenyang University of Technology. Her research interest is nanostructural metal oxide-based anode materials for lithium-ion batteries

        Xiaorui Hao Xiaorui Hao is currently a graduate student at Nanjing Tech University. Her research focuses on zinc-ion battery electrolytes and the interphase chemistry of electrodes/electrolytes

        Lin Li Lin Li is an Oujiang Distinguished Professor and associate dean of the Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University. He received his B.S. degree in materials science and engineering from Nanchang University (2016). He obtained his Ph.D. from Nankai University in 2021. His research focuses on advanced electrode materials and electrolytes for lithium-ion batteries, sodium-ion batteries, and potassium-ion batteries

        Chenglin Zhang Chenglin Zhang is currently a Jinshan Youth Distinguished Professor at Jiangsu University, China. He received his Ph.D. degree in Applied Physics from Institute of Physics, Technische Universität Ilmenau in 2022. His research mainly focuses on new electrochemical energy storage devices, such as sodium- and potassium-ion batteries, and hybrid ion capacitors

        Fanian Shi Fanian Shi received his Ph.D. in applied chemistry in 1996 at Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. He is currently a full professor at the Shenyang University of Technology and a member of the committee on Energy and Environment, China Energy Society. He specializes in the research of MOF composites for energy materials, photocatalysts, etc

        Yuhan Wu Yuhan Wu received his Ph.D. degree in material physics at the Ilmenau University of Technology in 2021. Since 2022, he has been an associate professor at the Shenyang University of Technology. His research interests focus on designing and synthesizing multiscale materials for energy conversion and storage

      • Corresponding author: linli@wzu.edu.cn; chenglinzhang@ujs.edu.cn; shifn@sut.edu.cn; yuhanwu@sut.edu.cn
      • Received Date: 2023-09-20
      • Revised Date: 2023-10-18
        • Available Online: 2023-11-13

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