Comparative study of pure and mixed phase sulfurized-carbon black in battery cathodes for lithium sulfur batteries

Surjit Sahoo, Debayan Chatterjee, Subhasish Basu Majumder, Kh M Asif Raihan, Brice LaCroix, Suprem R. Das
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Abstract

Lithium-sulfur battery (LSB) chemistry is regarded as one of the most promising contenders for powering next-generation electronics, including electric vehicles. This is due to its high theoretical capacity, the use of inexpensive and environmentally friendly materials, and its alignment with climate-smart manufacturing principles. Sulfur, the electroactive element in LSBs, undergoes lithiation to form a series of polysulfides, each contributing to the battery's energy density. However, this chemistry encounters several challenges, particularly concerning the stability of sulfur. Recent studies have shown that the presence of a full gamma phase of sulfur in an LSB cathode significantly enhances the capacity and overall cell performance. However, despite the advantages of cathodes with gamma sulfur, the characteristics of LSBs with mixed crystal phases of sulfur (alpha, beta, and gamma) have not been extensively studied. In this context, we developed a simple and cost-effective synthesis method to produce both single-phase (alpha) and mixed-phase sulfur (primarily a mixture of alpha and gamma, with a trace of beta) and conducted their detailed physical and electrochemical characterization for use as electroactive cathode materials in LSBs. The cells fabricated using sulfur-carbon black as the cathode delivered a specific capacity of approximately 640 mAh/g at a current density of 275 mA/g, demonstrating excellent cyclic stability over 50 cycles with a capacity retention of around 97%. This performance is superior to that of the sulfur-baked carbon black composite cathode, which achieved 440 mAh/g at the same current density.

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硫化锂电池正极中纯碳黑和混相硫化碳黑的比较研究
锂硫电池(LSB)化学被认为是为包括电动汽车在内的下一代电子产品提供动力的最有前途的竞争者之一。这得益于其理论容量高、使用廉价环保材料以及符合气候智能制造原则。LSB中的电活性元素硫会发生锂化反应,形成一系列多硫化物,从而提高电池的能量密度。然而,这种化学反应遇到了一些挑战,尤其是硫的稳定性。最近的研究表明,在 LSB 阴极中存在全伽马硫相可显著提高电池容量和整体性能。然而,尽管伽马硫阴极具有优势,但对具有混合硫晶相(α、β 和伽马)的 LSB 的特性还没有进行广泛的研究。在这种情况下,我们开发了一种简单而经济有效的合成方法来生产单相硫(α)和混合相硫(主要是α和γ的混合物,还有微量的β),并对它们进行了详细的物理和电化学表征,以用作 LSB 中的电活性阴极材料。使用硫碳黑作为阴极制造的电池在电流密度为 275 mA/g 时的比容量约为 640 mAh/g,在 50 个循环周期内表现出卓越的循环稳定性,容量保持率约为 97%。这一性能优于硫焙烧炭黑复合阴极,后者在相同电流密度下的比容量为 440 mAh/g。
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