High-quality Fe4[Fe(CN)6]3 Nanocubes: Synthesis and Electrochemical Performance as Cathode Material for Aqueous Sodium-ion Battery

doi:10.15541/jim20190076

Abstract

Abstract:

High-quality Fe₄[Fe(CN)₆]₃ (HQ-FeHCF) nanocubes were synthesized by a simple hydrothermal method. Its structure, morphology and water content are characterized. Fe₄[Fe(CN)₆]₃ exhibits regular cubic shape with a uniform size of ca. 500 nm, which belongs to the face-centered cubic phase. Fe₄[Fe(CN)₆]₃ shows discharge capacities of 124, 118, 105, 94, 83, 74 and 64 mAh·g ^-1 at 1C, 2C, 5C, 10C, 20C, 30C and 40C rate, respectively, in the aqueous ternary electrolyte of NaClO₄-H₂O-Polyethylene glycol. Its capacity retention remains 100% after 500 charge/discharge cycles at the rate of 5C. The full battery with Fe₄[Fe(CN)₆]₃ as cathode and NaTi₂(PO₄)₃ as anode was fabricated, which delivers a specific energy density of 126 Wh·kg ^-1 (based on the active electrode materials) with a voltage output of 1.9 V. Furthermore, 92% of its initial discharge capacity retains after 140 charge/discharge cycles at a rate of 5C, and its Coulomb efficiency is close to 100%.

Key words: aqueous sodium-ion battery, cathode material, cubic structure, energy density

CLC Number:

TQ174

WANG Wu-Lian, ZHANG Jun, WANG Qiu-Shi, CHEN Liang, LIU Zhao-Ping. High-quality Fe₄[Fe(CN)₆]₃ Nanocubes: Synthesis and Electrochemical Performance as Cathode Material for Aqueous Sodium-ion Battery[J]. Journal of Inorganic Materials, 2019, 34(12): 1301-1308.

Figures/Tables 11

Fig. 1 (a) XRD patterns and (b)TG curves of HQ-FeHCF and LQ-FeHCF with inset in (a) showing crystal structure of HQ-FeHCF

Table 1 Fractional coordinates of HQ-FeHCF determined from Rietveld method

Atom	Wyckoff position	x	Site occupancy
Fe₁	4a	0.0000	0.9790
Fe₂	4b	0.5000	0.8901
C	24e	0.2024	0.9771
N	24e	0.2988	0.9771

Table 2 Fractional coordinates of LQ-FeHCF determined from Rietveld method

Atom	Wyckoff position	x	Site occupancy
Fe₁	4a	0.0000	0.8458
Fe₂	4b	0.5000	0.6262
C	24e	0.2260	0.8420
N	24e	0.3275	0.8420

Fig. 2 SEM images of (a-b) HQ-FeHCF and (c-d) LQ-FeHCF

Fig. 3 TEM images of (a) HQ-FeHCF and (b) LQ-FeHCF

Fig. 4 (a) Cyclic voltammogram (CV) curves of HQ-FeHCF and LQ-FeHCF at the sweep rate of 1 mV·s-1 in the electrolyte of Na-H2O-PEG; (b) Charge and discharge curves of HQ-FeHCF and LQ-FeHCF at 1C; (c) Rate performance of HQ-FeHCF and LQ-FeHCF; (d) Cycling performance of HQ-FeHCF and LQ-FeHCF

Fig. 5 SEM images of HQ-FeHCF after (a-b)100 and (c-d) 500 cycles

Fig. 6 TG curves of HQ-FeHCF and LQ-FeHCF after 500 cycles

Fig. 7 Ex situ XRD patterns of HQ-FeHCF material at various states of charge and discharge

Fig. 8 (a) Cyclic voltammogram (CV) curves of HQ-FeHCF and NaTi2(PO4) at the sweep rate of 1 mV·s-1 in the electrolyte of Na-H2O-PEG; (b) Galvanostatic charge-discharge profiles at 1C for full cell, cathode, and anodein the electrolyte of Na-H2O-PEG; (c) Rate performance and (d) cycling performance of full cell

Table 3 Energy density of different aqueous sodium-ion batteries

Cathode	Anode	Energy density/ (Wh·kg^-1)	Ref.
Na_0.44MnO₂	NaTi₂(PO₄)₃	33	[39]
Na₂Ni[Fe(CN)₆]	NaTi₂(PO₄)₃	43	[13]
Na₂Cu[Fe(CN)₆]	NaTi₂(PO₄)₃	48	[40]
NaMnO₂	NaTi₂(PO₄)₃	30	[12]
K_0.27MnO₂	NaTi₂(PO₄)₃	55	[41]
NaFePO₄	NaTi₂(PO₄)₃	61	[42]
Na₂VTi(PO₄)₃	NaTi₂(PO₄)₃	68	[43]
Na₃MnTi(PO₄)₃	NaTi₂(PO₄)₃	82	[44]
Na_0.66Mn_0.66Ti_0.34O₂	NaTi₂(PO₄)₃	76	[45]
Na₂Ni_0.4Co_0.6[Fe(CN)₆]	NaTi₂(PO₄)₃	121	[46]
Fe₄[Fe(CN)₆]₃	NaTi₂(PO₄)₃	126	This work

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High-quality Fe₄[Fe(CN)₆]₃ Nanocubes: Synthesis and Electrochemical Performance as Cathode Material for Aqueous Sodium-ion Battery

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