Research Progress on Anode Materials and Interfacial Chemistry for Rechargeable Magnesium Batteries

doi:10.11900/0412.1961.2024.00357

Acta Metall Sin

2025, Vol. 61

Issue (3): 437-454 DOI: 10.11900/0412.1961.2024.00357

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Research Progress on Anode Materials and Interfacial Chemistry for Rechargeable Magnesium Batteries

WEN Tiantian¹^,², YUE Jili¹^,², XIONG Fangyu¹^,², YUAN Yuan¹^,², HUANG Guangsheng¹^,²(

), WANG Jingfeng¹^,², PAN Fusheng¹^,²

1 School of Materials Science and Engineering, Chongqing University, Chongqing 400044, China
2 National Engineering Research Center for Magnesium Alloys, Chongqing University, Chongqing 400044, China

Cite this article:

WEN Tiantian, YUE Jili, XIONG Fangyu, YUAN Yuan, HUANG Guangsheng, WANG Jingfeng, PAN Fusheng. Research Progress on Anode Materials and Interfacial Chemistry for Rechargeable Magnesium Batteries. Acta Metall Sin, 2025, 61(3): 437-454.

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Abstract

Rechargeable magnesium batteries have emerged as highly promising alternatives in the field of ion batteries, owing to their excellent electrochemical performance, abundance of magnesium resources, and uniform deposition of magnesium. However, challenges such as interface passivation, volume expansion, and uneven stripping/plating of anode materials persist in impeding the commercialization process of rechargeable magnesium batteries. Despite significant progress in exploring novel anode materials and interfacial chemical regulation strategies, developing anode materials that combine high energy density, high power density, excellent stability, and extremely long cycle life continues to pose numerous challenges. This study comprehensively and systematically reviewed the latest research on anode materials and interface regulations for rechargeable magnesium batteries. The influence of material composition, microstructure, and surface/interface structure on electrochemical properties and their underlying mechanisms were analyzed, along with the prospects for the future development and design of anode materials for magnesium batteries and interface regulation.

Key words: rechargeable magnesium battery anode material anode-electrolyte interface regulation strategy

Received: 25 October 2024

ZTFLH:

TM911

Fund: National Natural Science Foundation of China(U23A20555);Chongqing Technology Innovation and Application Development Project(2024TIAD-KPX0003)

Corresponding Authors: HUANG Guangsheng, professor, Tel: (023)65102821, E-mail: gshuang@cqu.edu.cn

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	WEN Tiantian
	YUE Jili
	XIONG Fangyu
	YUAN Yuan
	HUANG Guangsheng
	WANG Jingfeng
	PAN Fusheng

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https://www.ams.org.cn/EN/10.11900/0412.1961.2024.00357 OR https://www.ams.org.cn/EN/Y2025/V61/I3/437

Fig.1 Dilemmas of Mg anode
(a) passivation of Mg anode^[19] (b, c) uneven stripping/plating of Mg anode^[20,21] (DLA—diffusion-limited aggregation) (d) machining problem of Mg anode^[22,24] (RD—rolling direction)

Fig.2 Representative researches of Mg-Ga alloy anodes
(a) solid-liquid phase transformation and long cycle-life of Mg-Ga system^[25]
(b) morphologies of Ga confined by reduced graphene oxide (Ga@rGO) before and after charging process^[36]

Fig.3 Passivation mechanisms
(a) bond dissociation energy (BDE) of TFSI

-

, [Mg⁺-TFSI

-

], and [Mg²⁺-TFSI

-

]^[41]
(b) instability of the coordinated solvents^[42] (G1—monoglyme, G2—diglyme, G3—triglyme, DMS—dimethyl sulfone, TMS—tetramethylene sulfone, ACN—acetonitrile, E_red—reduction potentials)
(c) binding energy and charge state of solvated structure in electrolytes^[43]

Fig.4 Uneven Mg plating/stripping mechanism^[55]
(a) schematic of Mg electroplating progress and the standard parameters to guide the diffusion limited theory and the nucleation theory (take the all phenyl complex (APC) electrolyte as an example) (r_crit—critical radius, η_n—overpotential, γ—surface energy, F—Faraday's constant, V_m—molar volume, τ_Sand—Sand's time, i_L—limited current, C₀—salt concentration in bulk electrolyte, D_ambp—ambipolar diffusion coefficient, n—electron transfer number, A—electrode area, L—thickness, μ_a—anion transference number, μ_c—cationic transference number, D_c—self-diffusion coefficient of individual cation, D_a—self-diffusion coefficient of individual anion, t₊—cationic transference number. THF—tetrahydrofuran)
(b) diagram of diffusion-control buffer zone
(c) cross sectional SEM image and schematic of Mg deposit at 10 mA/cm² in APC electrolyte
(d) Mg plating in glass fiber separator at 5 mA/cm²

Fig.5 Volume expansions
(a) Mg@BP^[57] (Mg/black phosphorous composite anode)
(b) Bi-NTs nano structure anode^[34] (NTs—nanotubes)
(c) Bi-Sn multiphase alloy anode^[59] (d) InSb-10%C anode^[64]

Fig.6 Theoretical calculation of adsorption energy and diffusion energy
(a) calculated adsorption energies of Mg atoms onto different Mg and MgIn crystal facets^[65]
(b) adsorption models and energies of THF, glyme (DME), G2, and 2-methoxyethylamine (MOEA) molecules on Mg (0001)^[51](SEI—solid electrolyte interphase)
(c) calculated Mg migration energy barriers in bulk Mg₃Sb₂ and MgCl₂^[66]
(d) summary of the calculated diffusion barriers of Mg²⁺ in various inorganic Mg compounds^[67]

Fig.7 Phase-field and molecular dynamics (MD) simulation
(a) phase-field simulation morphologies of Li and Mg at different time under a constant potential of 0.1 V^[68] (r—distance between the calculate particle and the central particle)
(b) MD snapshots and radial distribution functions of O or N atoms in DME, G2, OTf, and MOEA with respect to Mg²⁺ in the Mg(OTf)₂/DME/G2 and Mg(OTf)₂/DME/G2/MOEA electrolytes, and solvation structure analysis of the two electrolyte systems^[44] (g(r)—radial distribution function)
(c) representative snapshots of Mg(TFSI)₂ and Mg[B(Otfe)₄]₂ on the Mg surface at various times from AIMD simulations at 750 K^[69]

Fig.8 Compositions and structure design of the anode materials
(a) 3D magnesiophilic anode materials^[70] (J / J₀—normalized current density, d / d₀—normalized electrode distance, E / E₀—normalized chemisorption energy, θ—wetting angle)
(b) nano-Mg (N-Mg) nanostructured anode^[71]
(c) AZ31 alloy anode^[72]
(d) Mg-Gd alloy anode^[74]
(e) Mg-Ce alloy anode^[76]

Fig.9 SEI fabricated anodes
(a) Mg₂Ga₅ alloy-type layer^[82]
(b) Ga₅Mg₂-Mg layer^[80]
(c) Bi/MgCl₂/PTHF (polytetrahydrofuran) SEI layer^[84] (ECH—epichlorohydrin)
(d) schematic illustration of the MgMOF@Mg^[87] (MOF—metal organic framework)
(e) zeolite-polymer SEI layer^[89]
(f) phytic acid (PA) SEI layer^[91]
(g) PA-Al SEI layer^[92]

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