Impact of nanoscale Prussian blue suspension electrolyte on the performance of lithium-oxygen batteries

doi:10.11949/0438-1157.20250024

Abstract

Abstract:

Prussian blue (PB) has attracted much attention in the field of electrochemical storage due to its three-dimensional frameworks. In this study, PB was dispersed into the electrolyte to form a stable suspension, allowing PB to co-deposit with discharge products during the discharge process of lithium oxygen batteries (LOBs). The high lithium-ion (Li⁺) migration number ( $t L i + =$ 0.67) offered by the incorporated PB accelerated the decomposition of discharge products and reduced the charging voltage. At the same time, the suspended PB promotes the homogenization of Li⁺ flux, which is beneficial to the uniform deposition and dissolution of lithium. Compared with the LiClO₄/DMSO electrolyte, the lifespans of lithium || lithium (Li||Li) symmetric batteries were extended from 257 h to 1000 h with 1.5 mg·ml^-1 PB suspension electrolyte, and the cycle numbers of LOBs were extended from 64 rounds to 430 rounds.

Key words: Prussian blue, nanomaterials, nanostructure, electrolytes, lithium protection, lithium-oxygen battery

摘要：

普鲁士蓝（PB）因其三维开放框架结构在电化学存储领域备受关注。将PB分散到电解液中形成稳定的悬浮液，使PB在锂氧电池（LOBs）放电过程中与放电产物共沉积，利用其高锂离子（Li⁺）迁移数（ $t L i + =$ 0.67）加速放电产物分解，降低充电电压；同时，悬浮的PB促进了Li⁺通量的均匀化，有利于锂的均匀沉积和溶解。与LiClO₄/DMSO电解液相比，添加1.5 mg·ml^-1PB悬浮电解液的锂||锂（Li||Li）对称电池的循环时间从257 h延长至1000 h，LOBs循环寿命从64圈延长到430圈。

关键词: 普鲁士蓝, 纳米材料, 纳米结构, 电解质, 锂保护, 锂氧电池

CLC Number:

TM 912

Aqiang WU, Xiangqun ZHUGE, Tong LIU, Mingxing WANG, Kun LUO. Impact of nanoscale Prussian blue suspension electrolyte on the performance of lithium-oxygen batteries[J]. CIESC Journal, 2025, 76(8): 4310-4317.

吴阿强, 诸葛祥群, 刘通, 王明星, 罗鲲. 纳米普鲁士蓝悬浮电解液对锂氧电池性能的影响[J]. 化工学报, 2025, 76(8): 4310-4317.

Figures/Tables 8

Fig.1 SEM image particle (a), size distribution (b), XRD analysis (c) of PB nanoparticles; Suspensibility of the PB/LiClO4/DMSO electrolytes with different PB contents (d)

Fig.2 Nyquist plot with different PB contents (a); EIS analysis of the PB1.5 electrolyte at 10 mV with a Li||Li symmetric cell (b)

Fig.3 Nyquist plots of the LOB cells with different electrolytes (a); Cyclic performance of the LOBs with different electrolytes [(b)—(e)]; Cut-off voltages at different cycles of LOBs with different electrolytes (f)

Fig.4 (a)Rate performance of the LOBs with PB0 and PB1.5; (b)Full-discharge capacities of LOBs

Fig.5 Cycling in the Li||Li symmetric cells at 0.1 mA·cm-2 with PB0 and PB1.5 (a); Li||Li symmetric cell cycle of a certain length of time after lithium surface SEM diagram [(b)—(d)]

Fig.6 SEM images of the MWCNTs cathodes (a); SEM images of LOBs with PB0 after the 1st discharge (b), the 1st recharge (c)and the 64th discharge (d); SEM images of LOBs with PB1.5 after the 1st discharge (e), the 1st discharge (f), the 200th discharge (g), the 430th discharge (h); Element mapping of the MWCNTs cathode after the 430th discharge in PB1.5-LOB [(i)—(l)]

Fig.7 Element mapping of the cathode after the 1st discharge in PB1.5-LOB

Fig.8 Surface SEM images of the Li negative electrodes with PB0-LOB (a) and PB1.5-LOB [(b)—(d)] at different cycles; XRD characterization of LOBs failed negative electrodes surface (e)

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