A Review of Metal Silicides for Lithium-Ion Battery Anode Application

doi:10.1007/s40195-020-01095-z

Abstract

Abstract:

Lithium batteries (LIBs) with low capacity graphite anode (~ 372 mAh g^-1) cannot meet the ever-growing demand for new energy electric vehicles and renewable energy storage. It is essential to replace graphite anode with higher capacity anode materials for high-energy density LIBs. Silicon (Si) is well known to be a possible alternative for graphite anode due to its highest capacity (~ 4200 mAh g^-1). Unfortunately, large volume change during lithiation and delithiation has prevented the Si anode from being commercialized. Metal silicides are a promising type of anode materials which can improve cycling stability via the accommodation of volume change by dispersing Si in the metal inactive/active matrix, while maintain greater capacity than graphite. Here, we present a classification of Si alloying with metals in periodic table of elements, review the available literature on metal silicide anodes to outline the progress in improving and understanding the electrochemical performance of various metal silicides, analyze the challenges that remain in using metal silicides, and offer perspectives regarding their future research and development as anode materials for commercial LIBs application.

Key words: Li-ion battery, Metal silicides, Anode materials, Electrochemical performance

Bo Ding, Zhenfei Cai, Zishan Ahsan, Yangzhou Ma, Shihong Zhang, Guangsheng Song, Changzhou Yuan, Weidong Yang, Cuie Wen. A Review of Metal Silicides for Lithium-Ion Battery Anode Application[J]. Acta Metallurgica Sinica (English Letters), 2021, 34(3): 291-308.

Figures/Tables 16

Fig. 1 Metal elements used for the formation of silicides in the M-Si system

Table 1 Typical silicides of elements in metal groups

Elements	Group	Product
Li	I	Li₂₂Si₅ Li₁₃Si₄ Li₇Si₃ Li₁₂Si₇ LiSi
Ca	II	Ca₂Si Ca₅Si₃ CaSi CaSi₂
Mg	II	Mg₂Si
Ti	III	Ti₃Si Ti₅Si₄ TiSi TiSi₂
Co	III	Co₂Si CoSi Co₂Si₃ CoSi₂
Fe	III	Fe₃Si Fe₅Si₃ FeSi FeSi₂
Mn	III	Mn₃Si Mn₅Si₂ MnSi MnSi₂
Ni	III	Ni₂Si Ni₃Si₂ NiSi NiSi₂
Cr	III	Cr₃Si Cr₅Si₃ CrSi CrSi₂
Cu	III	Cu₃Si Cu₁₅Si₄ Cu₅Si
Ag	III	Ag + Si
Al	IV	Al + Si
Sn	IV	Sn + Si
Ge	IV	Ge_1-_xSi_x (x = 0-1 at%)

Fig. 2 a IR spectra for samples C-1 and C-2 measured in air with the attenuated total reflectance (ATR) method. b Discharge capacity for samples C-1 and C-2 over 100 cycles evaluated at a constant current of 100 mA g-1 with a voltage window of 0.02-1.5 V (vs. Li/Li+). The commercial sample is an Mg2Si reagent powder with particle diameters less than 53 μm [27]

Fig. 3 a Cycling performance of Pure Mg2Si. b Rate performance of carbon-coated Mg2Si electrode at different current density. c Cycling performance of carbon-coated Mg2Si with its corresponding coulombic efficiency measured at 100 mA g-1 [28]

Fig. 4 a SEM images of a vertically aligned Si/Ge nanotube array on a stainless steel substrate. b Magnification TEM images of a single Si/Ge nanotube. Inset of b shows selective area electron diffraction pattern. c Cycle performances. d Rate capabilities of Si nanotube and Si/Ge nanotube array electrodes at various C rates [31]. e Charge and discharge capacities (mAh g-1) of Si-Ge heterostructure nanowires demonstrated at different current rates. f Overview of the synthetic protocol used to prepare Sn-seeded Si-Ge hNWs directly from current collectors and the changes in morphology due to repeated cycling with Li from segmented crystalline structures to an amorphous alloyed network after 50 cycles [33]

Fig. 5 a The schematic illustration for the growth process of the Si-NiSix nanocomposites. b TEM image of an individual a-Si/NiSix nanowire. The inset shows a plan-view SEM image of a-Si/NiSix grown on substrate. c HRTEM image of an individual a-Si/NiSix nanowire at the core region and the corresponding electron diffraction pattern (inset). d The discharge capacity for the a-Si/NiSix nanowire and the a-Si/c-Si nanowire, respectively. e The rate capability for the a-Si/NiSix nanowire and the a-Si/c-Si nanowire, respectively [59]

Fig. 6 a The schematic drawing of the ball milling and the calcining process for the preparation of FSO anode materials. b Cycling property of the FSO-800 °C electrode [64]

Fig. 7 Preparation process of the HCS NW structure grown overall on the copper foam substrate. A schematic illustration of the preparation of the HCS NW hybrid structure. a Copper foam. b and c Crossing CuO NWs grown on the CuO foam after thermal oxidation growth in atmosphere. d Interconnected CuO/a-Si core-shell NWs after coating the a-Si layer. e Sn-catalyzed Si NWs were grafted on the front and back plates of the CuO/a-Si core-shell NW foam, respectively, and finally obtained hierarchical nano-branched c-Si/CuO@a-Si core shell NW structures grown overall on the foam substrate in the PECVD system. f The hierarchical Cu-Si NW hybrid structure grown on the copper foam after a high temperature H2 annealing process. g ALD-coated ultra-thin Al2O3 on the hierarchical Cu-Si NW structure, and the corresponding image enlarged for detail. h Schematic diagram and photographs of the front and back plates of the HCS hybrid structure. i Photographs of a water droplet and j an electrolyte droplet on the surface of the HCS NW hybrid structure. k Cycling rate performance of the HCS NW hybrid anode with a mass loading of 1.2 mg cm-2. l Ultra-long-term cycling performance for ICS NT trunks (interconnected Cu-Si alloy nanotube trunks) at 20 A g-1 [69]

Fig. 8 a, b The capacities of C49 TiSi2 nanonets and ordinary C54 TiSi2 nanowires at a current density of 1000 mA g-1, respectively. Insets: corresponding SEM pictures of the nanonets and nanowires, respectively. c Charge capacity and Coulombic efficiency of TiSi2 nanonets with oxide coating at a rate of 2000 mA g-1. Potential range: 1.0-0.01 V. Inset: Schematic and TEM images for clearly understand of TiSi2 nanonets with oxide coating. d A TEM picture manifests the particulate nature of the Si coating on TiSi2 NNs. e Charge capacity and Coulombic efficiency of the Si/TiSi2 heteronanostructure at a rate of 8400 mA g-1 tested between 0.150 and 3.00 V. Inset: schematic of the Si/TiSi2 heteronanostructure. f Structure of Si-Ti framework and its electrochemical performance [72, 75, 77]

Fig. 9 Comparison of the cycle performances of the Si/NiTi alloy and pure Si electrodes between 2.0 and 0.0 V (vs. Li/Li+) at a cycling rate of 100 mA g-1 with coulombic efficiency. Inset: schematic microstructure of the Si/Ni-Ti matrix alloy [81]

Fig. 10 a Schematic illustration of the nano-Si/FeSi2Ti heterostructure during lithiation. b HRTEM images of the nano-Si/FeSi2Ti heterostructure after 50 cycles. c The cyclic retention of the nano-Si/FeSi2Ti heterostructure and Si nanoparticles at 0.1 C. d The dependence of discharge retention on the variation of current density for galvanostatic charge-discharge [87]

Fig. 11 a HRTEM image of the layered zinc silicate/C composited nanomaterials. b Reversible charge capacities of the above electrodes cycled at various rates (50-1000 mA g-1) [97]

Table 2 Electrochemical performance of some metal silicides

Materials	Discharge plateaus (V)	Initial coulomb efficiency (%)	Cycling stability (current rate, specific capacity, cycle numbers, capacity retention)	References
Mg₂Si	0.01-3.0	84.0	100 mAh g^-1, 1040 mAh g^-1, 35 cycles, 4.0%	[26]
Mg₂Si/C	0.02-2.0	60.6	100 mAh g^-1, 1199 mAh g^-1, 500 cycles, 39.2%	[28]
Ge_0.1Si_0.9	0.02-2.0	94.0	0.8 mA g^-1, 2022.12 mAh g^-1, 100 cycles, 52.8%	[30]
Ge_0.25Si_0.75	0.02-2.0	95.0	0.8 mA g^-1, 1992.10 mAh g^-1, 100 cycles, 62.8%	[30]
Ge_0.5Si_0.5	0.02-2.0	98.0	0.8 mA g^-1, 1934.12 mA g^-1, 100 cycles, 64.3%	[30]
Si/Ag/C	0.005-3.0	61.9	200 mAh g^-1, 988 mAh g^-1, 10 cycles, 71.0%	[102]
Si/Ni	0.0-2.0	82.4	233 mA g^-1, 650 mAh g^-1, 100 cycles, 72.9%	[57]
Si₈₀Ni₂₀	0.0-2.0	59.0	50 mAh g^-1,1304 mAh g^-1, 15 cycles, 7.7%	[56]
Si₇₀Ni₃₀	0.005-2.0	80.9	240 mAh g^-1, 600 mAh g^-1, 30 cycles, 90%	[103]
NiSi₂/Si/C	0.01-1.1	81.0	2034 mAh g^-1, 765 mAh g^-1, 200 cycles, 86.7%	[100]
MP-Si/Ni/C	0.01-1.5	68.2	200 mAh g^-1, 1942.4 mAh g^-1, 120 cycles, 57.3%	[104]
Fe₁₄Si₈₆	0.02-1.5	92.0	100 mAh g^-1, 1528 mAh g^-1, 100 cycles, 34.8%	[98]
Fe₁₀Si₉₀-G-C	0.0-2.0	87.0	200 mAh g^-1, 1201 mAh g^-1, 80 cycles, 88.5%	[105]
Fe₂₀Si₄₀-G	0.0-1.2	84.0	-, 800 mAh g^-1, 20 cycles, 75.0%	[63]
Si-Cu₃Si	0.0-1.5	93.5	100 mAh g^-1, 1310 mAh g^-1, 30 cycles, 83.0%	[106]
Si-Ti	0.02-1.5	77	0.1 mA cm^-3, 1542 mAh g^-1, 50 cycles, 15.3%	[107]
Si-Mn/rGO	0.01-3.25	64.6	100 mAh g^-1, 1033 mAh g^-1, 50 cycles, 57.6%	[108]
Si/Co-CoSi₂	0.01-3.0	77.9	100 mAh g^-1, 1200 mAh g^-1, 80 cycles, 79.3%	[109]

Fig. 12 Electrochemical performance of some metal silicides

Table 3 Electrochemical performance of different nanostructured metal silicides

Type of silicide	Nanostructure	Capacity (mAh g^-1)	Cycle	Capacity retention (%)	Current density	References
Si_0.5Ge_0.5	Mixed particles	2022.12	100	64.3	0.8 mA g^-1	[30]
Si/Ge	Nanotube	2362	100	24.8	200 mAh g^-1	[110]
cpSG@C (canyon-like Si-Ge alloy@C)	Nanoparticles with canyon-like surface	1247	100	78.3	500 mAh g^-1	[111]
Si₅₃Ge₄₇	Core-shell	1692	60	90.0	5C	[112]
Si_0.67Ge_0.33	Nanowires	1709	250	79.6	C/5	[32]
Si/Ge	Heterostructure nanowires	1644	400	71.8	C/5	[33]
Ni₃Si/Si/NWs	Core-shell	3773	50	71.0	2.1 A g^-1	[113]
Ni_xSi_y	Core-shell nanowire	1406	100	73.7	1 A g^-1	[114]
NiSi_x/a-Si	Nanowire	1400	150	87.3	10 A g^-1	[115]
Ni/Si	Core/shell nanosheet	2905	100	87.0	C/2	[116]
Ni₂Si/Si	Core-shell	1547	600	85.0	358 mA g^-1	[117]
3DGF/Cu/Si (three-dimensional graphene foam/Cu/Si)	Core-shell nanoflowers	1647	500	65.1	3.2 A g^-1	[118]
Si-Cu	Nanotubes	780	1000	88.0	20 A g^-1	[68]
Cu-Si	Core-shell nanotube arrays	2473	400	60.9	C/2	[119]
HCS NW (hierarchical Cu-Si nanowire)	Nanowire hybrids	800	9000	60.0	20 A g^-1	[69]
Si₈₀Ti₂₀	Thin film	1017	300	≈ 100	2 A g^-1	[120]
Si-Ti	Binary framework	960 (2nd)	200	82.1	2 A g^-1	[77]

Fig. 13 Schema of a classification of metal silicides, corresponding challenges and solutions

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