Key Takeaways & Executive Findings
- •• An integrated conjugated microporous polymer composite electrode (C4N/rGO) with high conductivity, large specific surface area and good solvent resistance was prepared by in-situ growth. • An antifreeze alkaline electrolyte (0.1 DMSO/2 M NaOH) was developed to broaden the operation temperature zone and voltage window of the aqueous alkaline battery. • The prepared aqueous alkaline battery exhibits a high energy density (147.3 Wh Kg−1 at 25 °C), outstanding long cycling stability and excellent wide-temperature-range performance (−70 to 45 °C). • The C4N/rGO//Ni(OH)2 full cell demonstrates ultra-high cycling stability over 38,000 cycles, offering a promising solution for extreme-condition energy storage.
Abstract
Common anode materials in aqueous alkaline electrolytes, such as cadmium, metal hydrides and zinc, usually suffer from remarkable biotoxicity, high cost, and serious side reactions. To overcome these problems, we develop a conjugated porous polymer (CPP) in-situ grown on reduced graphene oxide (rGO) and Ketjen black (KB), noted as C4N/rGO and C4N/KB respectively, as the alternative anodes. The results show that C4N/rGO electrode delivers a low redox potential (−0.905 V vs. Ag/AgCl), high specific capacity (268.8 mAh g−1 at 0.2 A g−1), ultra-stable and fast sodium ion storage behavior (216 mAh g−1 at 20 A g−1) in 2 M NaOH electrolyte. The assembled C4N/rGO//Ni(OH)2 full battery can cycle stably more than 38,000 cycles. Furthermore, by adding a small amount of antifreeze additive dimethyl sulfoxide (DMSO) to adjust the hydrogen bonding network, the low-temperature performance of the electrolyte (0.1 DMSO/2 M NaOH) is significantly improved while hydrogen evolution is inhibited. Consequently, the C4N/rGO//Ni(OH)2 full cell exhibits an energy density of 147.3 Wh Kg−1 and ultra-high cycling stability over a wide temperature range from −70 to 45 °C. This work provides an ultra-stable high-capacity CPP-based anode and antifreeze electrolyte for aqueous alkaline batteries and will facilitate their practical applications under extreme conditions.
1. Introduction
In recent years, rechargeable batteries have received widespread attention as an efficient energy storage system to meet the development needs of a green economy in society [1]. Sodium is 440 times more abundant than lithium in the Earth’s crust and is widely distributed and simple to extract [2]. Considering the abundance of the element and the cost of the resource, sodium has appeared as a substitute for lithium in recent years and has gained more and more attention in the field of batteries [3–6]. Aqueous rechargeable batteries have low cost, high safety and reliability, and fast kinetics compared with the organic electrolyte-based batteries, which meet the needs of modern green economy development [7, 8]. Therefore, the interest in aqueous rechargeable batteries is increasing day by day.
Conventional electrolytes for aqueous rechargeable batteries are commonly H2SO4 for acidic batteries [9], alkali metal salts (Li+, Na+) for neutral batteries [10], and MOH (M = alkali metal) for alkaline batteries [11]. Aqueous alkaline batteries are the latent high energy rechargeable batteries with prospects for large-scale energy storage applications [12]. Commercial aqueous alkaline batteries usually used nickel-based cathode (Ni(OH)2, theoretical specific capacity 289 mAh g−1) and metal or alloy anodes (zinc, iron, cadmium, hydrogen storage alloys, etc.) [13]. In 2022, Zhou et al. reviewed nickel-based rechargeable aqueous alkaline batteries such as Ni–Fe, Ni–Cd, Ni–MH, and Ni–Zn, and recounted their advantages and operating principles [14]. Since the anode materials of aqueous alkaline batteries always have some shortcomings [11], it is the quest of researchers to find anode materials with low cost, environmental friendliness, high specific capacity and suitable redox potentials [15–17].
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Mengxiao Li, Rui Li, Huige Ma, Mingsheng Yang, Yujie Dai, HaiPing Yu, Yuxin Hao, Zhihui Wang, Bei Wang, Mingjun Hu, Jun Yang (2025). An Ultra-Stable, High-Energy and Wide-Temperature-Range Aqueous Alkaline Sodium-Ion Battery with the Microporous C4N/rGO Anode. Nano-Micro Letters. https://doi.org/10.1007/s40820-024-01589-w
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Frequently Asked Questions
What is the main innovation of this paper?
The paper introduces a novel C4N/rGO composite anode for aqueous alkaline sodium-ion batteries, combined with an antifreeze electrolyte (0.1 DMSO/2 M NaOH), enabling ultra-stable cycling and operation over a wide temperature range from -70 to 45 °C.
What are the key performance metrics of the C4N/rGO anode?
The C4N/rGO anode delivers a low redox potential (-0.905 V vs. Ag/AgCl), high specific capacity (268.8 mAh g−1 at 0.2 A g−1), and excellent rate capability (216 mAh g−1 at 20 A g−1) in 2 M NaOH electrolyte.
How does the antifreeze electrolyte improve low-temperature performance?
The addition of dimethyl sulfoxide (DMSO) adjusts the hydrogen bonding network of the electrolyte, significantly improving low-temperature performance while inhibiting hydrogen evolution, thus enabling operation at temperatures as low as -70 °C.
What is the cycling stability of the full battery?
The assembled C4N/rGO//Ni(OH)2 full battery can cycle stably for more than 38,000 cycles, demonstrating ultra-high cycling stability.
What is the energy density of the full cell?
The full cell exhibits an energy density of 147.3 Wh kg−1 at 25 °C, which is high for aqueous alkaline batteries.
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