Promoting ion adsorption and desolvation kinetics enables high capacity and rate capability of stibium anode for advanced alkaline battery

doi:10.1016/j.jmst.2022.05.024

Abstract

Abstract:

Stibium (Sb) metal with high theoretic capacity, suitable negative working window and inexpensive nature are promising anode material for advanced aqueous alkaline batteries (AABs). However, the further development of Sb anode is severely hindered by the low capacity and poor rate capability which is originated from deficient adsorption of [Sb(OH)₄]⁻ and its sluggish desolvation kinetics. Herein, a nitrogen doped carbon cages (NCCs) substrate is constructed as high capacity and rate capability anode by promoting the adsorption and following desolvation process of [Sb(OH)₄]⁻ via the enhanced attraction toward (OH)⁻ in the solvated [Sb(OH)₄]⁻. Consequently, the designed Sb/NCCs anode delivers a high capacity of 627 mAh g⁻¹ with an average 95% Sb utilization, an outstanding coulombic efficiency (CE) of 95% and an impressive lifespan (>110 h). Meanwhile, the Ni₃Se₂//Sb/NCCs batteries show great capacity retention of 86.7% after 2000 cycles with an areal capacity of 0.52 mAh cm⁻². Implementation of the designed anode allows for the construction of Sb-based AABs with enhanced rate capability, energy density and cycling performance.

Key words: Aqueous alkaline batteries, Stibium anode, N-doped carbon, Ion adsorption, Desolvation kinetics

Peng Zhang, Jinhao Xie, Fan Yang, Xin Shi, Yanxia Yu, Xihong Lu. Promoting ion adsorption and desolvation kinetics enables high capacity and rate capability of stibium anode for advanced alkaline battery[J]. J. Mater. Sci. Technol., 2022, 131: 60-67.

Figures/Tables 5

Fig. 1. Schematic illustration of (a) NCCs and (b) CCs surfaces during the charging-discharging process.

Fig. 2. (a) TEM images of NCCs (inset is SEM images of NCCs). (b) N 1 s and (c) O 1 s XPS spectra of CCs and NCCs. Voltage profiles of CCs and NCCs at 10 mA cm?2 under a fixed capacity of (d) 1 mAh cm?2 and (e) 2 mAh cm?2. (f) Capacity comparisons between Sb/NCCs and recently reported anodes for AABs. (g) CE of the Sb plating/stripping process on CCs and NCCs electrode at 1 mAh cm?2 and 2 mAh cm?2 with a fixed current density of 10 mA cm?2. (h) Voltage gap of CCs and NCCS electrodes at different current densities with the capacity limited to 1 mAh cm?2.

Fig. 3. SEM images of Sb deposition with a capacity of 0.5, 2, and 5 mAh cm?2 at a current density of 10 mA cm?2 on CCs (a-c) and NCCs (e-g). Cross-sectional SEM images of Sb deposition on a bare CCs electrode (d) and an NCCs electrode (h) at 10 mA cm?2 to an areal capacity of 2 mA h cm?2. (i) Particle size distribution on NCCs electrode at 0.5 mAh?cm?2. (j) Voltage-time curves during Sb nucleation at 10 mA cm?2 on CCs and NCCs electrodes. (k) Schematic diagram illustrating the ion/electron transport in metal stripping.

Fig. 4. (a) Binding energies of [Sb(OH)4]? with different types of oxygen functional groups on CCs and NCCs by density functional theory (DFT) calculations. 3D charge difference between (b) CCs and (c) NCCs electrode and [Sb(OH)4]? with C-OH as adsorption sites. (d) Sb3+ ion contents in 5% v/v HNO3 solution after [Sb(OH)4]? adsorption experiment. (e) Binding energies between bare C, different types of nitrogen doped C and Sb. Schematic illustration of [Sb(OH)4]? desolvation and subsequent deposition in (f) CCs and (g) NCCs electrode. Arrhenius behavior of the resistance corresponding to (h) [Sb(OH)4]? desolvation and (i) Sb3+ plating.

Fig. 5. (a) CV curves of the Ni3Se2 cathode and Sb/FCS anode measured at 10 mV s?1. (b) GCD curves of Ni3Se2//Sb/NCCs battery at different current densities. (c) Areal capacities and (d) cycling performance of Ni3Se2//Sb/CCs and Ni3Se2//Sb/NCCs batteries. (e) Ragone plots of Ni3Se2//Sb/NCCs battery in comparison with advanced AABs.

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