Strategies Concerning Anode Modification in Rechargeable Magnesium Batteries

doi:10.7503/cjcu20210013

Abstract

Abstract:

Rechargeable magnesium batteries（RMBs） are a promising candidate for the development of high-energy storage systems due to its superiorities of relatively high theoretical volumetric capacity， high crustal abundance， low cost， especially environmental friendliness and safety. It is worth noting that the formation of a passivation film on the surface of magnesium（Mg） anode in most conventional electrolytes is an enormous obstacle， which leads to irreversible deposition/stripping behavior of Mg and thus limits the implementation of commercial RMBs. Researches focusing on electrolytes to tackle the obstacle have been in the bottleneck due to the restrictions of expensive price， complex synthesize process， low ionic conductivity， poor compatibility with cathodes and anodes simultaneously， etc. Facilitating modification of anode coming back to conventional electrolytes in RMBs is an alternatively promising avenue. This review summarizes recent studies concerning anode modification including alloy anode materials and formation of artificial interphase. Based on the analysis and comparison of previous researches， we propose conclusion and perspective for further development of RMBs.

Key words: Rechargeable magnesium battery, Alloy anode, Artificial interphase, Conventional electrolyte

CLC Number:

O646

TrendMD:

XUE Linlin, LYU Ruijing, WANG Aoxuan, LUO Jiayan. Strategies Concerning Anode Modification in Rechargeable Magnesium Batteries[J]. Chem. J. Chinese Universities, 2021, 42(5): 1357.

Figures/Tables 16

Table 1 Different properties of various metal anodes

Metal anode	Electrode potential/V	Gravimetric capacity/ (mA·h·g^-1)	Volumetric capacity/(mA·h·cm^-3)	Cost/(USD·kg^-1)	Abundance rank
Li	-3.04	3862	2066	19.2	33rd
Na	-2.71	1166	1128	0.2	6th
K	-2.93	685	591	1.0	7th
Mg	-2.37	2205	3832	2.2	8th
Zn	-0.76	820	5854	2.2	25th
Ca	-2.87	1337	2072	2.4	5th
Al	-1.66	2980	8046	1.9	3rd

Fig.1 Schematic of the passivation obstacle and modification strategies for RMBs

Fig.3 Electrochemical performance and illustration of structural transformation for Bi?Mg alloy anode[41](A) Cyclic voltammograms of Mg2+ insertion/deinsertion in Bi?NT and Bi?micro; (B) discharge/charge profile of a Mg?Bi cell; (C) rate performance of a Mg?Bi cell; (D) cycling stability and Coulombic efficiency of Bi electrode; (E) schematic illustration of the structural transformations of Bi?NT and Bi?micro during the discharge/charge process.Copyright 2013, American Chemical Society.

Fig.4 Electrochemical performance and XRD patterns of Sn?Mg alloy anode[48](A) 1st cycle galvanostatic magnesiation/demagnesiation curves for Sn/Mg and Bi/Mg half cells at 0.002C rate(using organohaloaluminate electrolyte); (B) magnesiation/demagnesiation capacities for Sn/Mg and Bi/Mg half?cells at various rates. Inset of (B): 10 cycles of a Sn/Mg half?cell at 0.005C and 0.01C rates in the same electrolyte; (C) the first 10 cycles for [Mo6S8/conventional electrolyte/Mg2Sn] and [Mo6S8/organohaloaluminate electrolyte/Mg2Sn] full?cell. Inset of (C): 1st cycle voltage profiles for each full?cell; (D) XRD patterns of demagnesiated Mg2Sn from organohaloaluminate and conventional electrolytes.Copyright 2013, The Royal Society of Chemistry.

Fig.5 Synthesis process and electrochemical performance of Sn based anode(A) Schematic illustration of process producing nanostructured Sn[50]; (B) capacity retention of Mg2Sn/APC/Mg cells following application of oxidative pulses and past the preconditioning steps at C/5 and C/2[50]; (C) cycling performance of micro?Sn[51]; (D) nano?Sn at C/20 in Mg half?cell using 0.5 mol/L PhMgCl/THF and 0.5 mol/L EtMgCl/THF as electrolyte respectively[51].(A, B) Copyright 2018, American Chemical Society; (C, D) Copyright 2018, MDPI AG.

Table 2 Specific properties of representative alloy anodes

Alloy element	Theoretical capacity/ (mA·h·g^-1)	Cost/ (USD·kg^-1)	Abundance	Reversibility/toxicity/ volume expansion	Conventional electrolyte	Ref.
Bi	Mg₃Bi₂ 385	28.3	4.8×10^-2 ppm	Reversible/Toxic	Mg(TFSI)₂/AN	[36]
					Mg(BH₄)₂?LiBH₄/diglyme	[41]
Sn	Mg₂Sn 900	18.0	2.2 ppm	Reversible/Non?toxic/120%	Mg(TFSI)₂/DME	[48]
Ga	Mg₅Ga₂ 1920	2200.0	18.0 ppm	Reversible/Non?toxic	Mg(TFSI)₂/AN	[61]
Ge	Mg₂Ge 1475	1200.0	1.8 ppm	Almost irreversible/Non?toxic/178%	―	[53]
Sb	Mg₃Sb₂ 660	4.4	0.2 ppm	Almost irreversible/Toxic	Mg(TFSI)₂/diglyme	[60]
Si	Mg₂Si 3817	1.4	27.7%	Maybe irreversible/Non?toxic/216%	―	[54,59]
Pb	Mg₂Pb 517	0.2	14.0 ppm	Reversible/Toxic	―	[55]
In	Mg₃In 1400	540.0	4.9×10^-2 ppm	Reversible/Toxic	―	[56]
P	Mg₂P 3461	300.0	1000.0 ppm	Maybe reversible/Non?toxic for black P	―	[57]
Al	Mg₁₇Al₁₂ 2582	2.0	8.1%	Maybe irreversible/Non?toxic	―	[58]

Fig.6 Mechanism and electrochemical performance of Ga?Mg alloy electrodes[61](A) Equilibrium phase diagram of the Mg?Ga system; (B) schematic of the magnesiation and demagnesiation process during which liquid Ga is reversibly converted into solid Mg2Ga5 at constant temperature and pressure; (C) long cycle?life of Mg2Ga5 alloy?type anode operating at 40 ℃ and 3C, 40 ℃ and 2C, 20 ℃ and 3C, 20 ℃ and 2C; (D) investigation of the compatibility of Mg2Ga5 with conventional electrolytes.Copyright 2019, Wiley?VCH.

Fig.7 Structure of the interphase and electrochemical performance of coated or bare Mg anodes[64](A) Schematic of a Mg powder electrode coated with the artificial Mg2+?conducting interphase, and the proposed structure for the interphase; (B) reversible Mg deposition/stripping in APC electrolyte; (C) voltage hysteresis versus cycle numbers for symmetric Mg electrodes with 0.5 mol/L Mg(TFSI)2/PC electrolyte; (D) voltage profiles of full cells using V2O5 as cathode in 0.5 mol/L Mg(TFSI)2/PC electrolyte; (E) reversible Mg deposition/stripping in 0.5 mol/L Mg(TFSI)2/PC electrolyte.Copyright 2018, Springer Nature.

Fig.8 Morphology characterization and electrochemical performance of pristine and Sn based Mg anodes[65](A) Schematic showing the Mg deposition behavior in Mg(TFSI)2/DME electrolyte with ionic transport interphase on Mg metal anodes; (B, C) surface views of the pristine Mg anode(0.05 mA/cm2)(B) and modified Mg anode(2 mA/cm2) plated with 2 mA·h/cm2 of Mg(C); (D, E) cross?sectional image for modified Mg anode plated with 2 mA·h/cm2(D) and the corresponding EDS mappings of Sn, Mg and Cl, respectively(E); (F) voltage profiles in symmetric cells with modified Mg anodes at a current density of 6 mA/cm2; (G) galvanos?tatic voltage profiles of the pristine and modified Mg anodes paired with TiS2 cathode at a current density of 10 mA/g.Copyright 2019, Oxford University Press.

Fig.9 Formation and operating mechanism of MgF2 interphase and electrochemical performance of fresh or coated Mg anodes[66](A) Schematic illustration of the formation process of the MgF2 surface coating; (B) schematic of the operating mechanism of the MgF2 for stripping and deposition of Mg metal; (C, D) schematics of failure mechanism for the Mg metal anode; (E) cross?section EDS mapping of as?prepared MgF2@Mg electrode; (F) voltage profiles of the symmetric cells cycling of fresh Mg and MgF2 coated Mg at current density of 0.25 mA/cm2; (G, H) voltage profiles(with Bi as cathode) of fresh Mg(G) and MgF2@Mg(H) at 120 mA/g.Copyright 2019, Elsevier.

Fig.10 Electrochemical performance of Mg anodes in electrolytes with or without I2 additive[68](A) Potential of Mg electrode during cycling in 0.5 mol/L Mg(TFSI)2/DME electrolytes with different amounts of I2 additive; (B) overpotentials for deposition and stripping; (C―F) EIS of Mg electrodes cycled in blank electrolyte and electrolytes with different concentrations of I2 additive.Copyright 2017, Wiley?VCH.

Fig.11 Operating mechanism of interphase and electrochemical performance of anodes in electrolytes with or without GeCl4 additive[69](A) Schematic diagrams showing the passivation layer in blank electrolyte; (B, C) breaking process for protection layer(B) and breaking and self?repair process for in situ?formed protection layer(C) during Mg deposition/stripping in conventional organic electrolyte; (D, E) cross?section SEM image(D) and the corresponding EDX mapping analysis(E) of the Ge?based protection layer; (F, G) voltage responses of symmetric Mg cells under repeated polarization from 1/4 h charge/discharge cycling at 0.02 mA/cm2(F) and 1/2 h charge/discharge cycling at 10 mA/cm2(G).Copyright 2019, Elsevier.

Fig.12 Mechanism of SEI formation and electrochemical performance of anodes in MBhfip/DME or LBhfip/DME electrolyte[70](A, B) The specific mechanism of SEI formation on the Mg anode surface in MBhfip/DME electrolyte(A) and LBhfip/DME electrolyte(B); (C) long?term cycling behavior of the Mg/Mg symmetrical cell(with LBhfip/DME) at the current density of 1.0 mA/cm2; (D) polarization behavior of the Mg/Mg symmetric cell with bare Mg electrodes and SEI protecting Mg electrodes at the current density of 0.1 mA/cm2 in Mg(TFSI)2/DME electrolyte; (E) charge?discharge profiles of Mo6S8/Mg battery(with LBhfip/DME electrolyte) at diffe?rent rates; (F) cycling stability and corresponding Coulombic efficiency of this Mo6S8/Mg battery for 6000 cycles at the rate of 10C.Copyright 2019, Wiley?VCH.

Fig.13 Operating mechanism of the tailored interphase on Mg anode and electrochemical performance in conventional electrolytes[71](A) Native passivation oxide layers on Mg anode; (B) artificial Mg2+?conducting layers tailored by SO2 chemisorption; (C) DFT calculation results for the energetics of Mg dissociation and migration with surface chemisorption structures; (D, E) top view of the calculated models of the mono?(D) and di?SO2 cases(E); (F) galvanostatic voltage profiles of Mg symmetric cells at 0.01 mA/cm2; (G) nyquist plots for Mg symmetric cells.Copyright 2020, American Chemical Society.

Fig.14 Comparison of artificial interphase formed in advance and in situ

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