掺杂氮的碳包覆 Ti1-xCoxN 纳米线作为多功能分离器与高供体数溶剂激活自由基介导的途径并促进 Li2S 转化,从而实现先进的锂硫电池

Gwan Hyeon Park, Won-Gwang Lim, Yun Ho Jeong, Song Kyu Kang, Minho Kim, Junhyuk Ji, Jungseub Ha, Sandya Rani Mangishetti, Subin Kim, Yeji Park, Changshin Jo, Won Bae Kim
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摘要

为了提高硫的利用率,有必要使用高供体数溶剂对电解质进行改性,但这种溶剂与锂金属的兼容性较差。应优化溶剂的用量,以最大限度地提高硫在阴极的利用率,并尽量减少与锂金属在阳极的副反应。与 DME/DOL 和 DMA/DOL 相比,1vol% N,N-二甲基乙酰胺(DMA)与 1,2-二甲氧基乙烷(DME)/1,3-二氧戊环(DOL)共溶剂的电解质溶液提高了放电容量,降低了过电位。除了对电解质进行改性,从高供体数溶剂中创建以自由基为介导的途径外,还通过有效减轻穿梭效应和利用高效电催化剂增强反应动力学来实现长周期性能。在 TiN 中掺入钴会使具有铁磁性的 d 带中心上移,从而抑制穿梭效应,激活以自由基为媒介的途径,促进 Li2S 的转化。通过电解质和电催化剂改性的协同作用,在 1 vol% DMA 电解质下用掺杂 N 的碳嵌入掺钴氮化钛纳米线(NC-Ti0.95Co0.05N NWs)制造的多功能分离器在 200 个循环后仍能达到 464.4 mA h g-1 的放电容量,衰减率为 0.093%/循环。这项工作凸显了具有高供体数溶剂的铁磁催化剂对锂硫(Li-S)电池的重要性。
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Activation of the Radical-Mediated Pathway and Facilitation of the Li2S Conversion by N-Doped Carbon-Embedded Ti1–xCoxN Nanowires as a Multifunctional Separator with a High Donor-Number Solvent toward Advanced Lithium–Sulfur Batteries
Electrolyte modification with a high donor-number solvent is necessary to increase sulfur utilization, but it also presents poor compatibility with lithium metal. The amount of the solvent should be optimized to maximize sulfur utilization at the cathode and minimize side reactions with Li metal at the anode. An electrolyte solution comprising 1 vol% N,N-dimethylacetamide (DMA) in a 1,2-dimethoxyethane (DME)/1,3-dioxolane (DOL) co-solvent demonstrated increased discharge capacity and reduced overpotential compared to DME/DOL and DMA/DOL. In addition to electrolyte, modification that creates radical-mediated pathways from a high donor-number solvent, long-cycle performance is achieved by effectively mitigating the shuttling effect and enhancing reaction kinetics with an efficient electrocatalyst. Cobalt doping into TiN introduced an upshift of the d-band center with ferromagnetic properties that suppressed the shuttling effect, activated radical-mediated pathways, and facilitated the Li2S conversion. A multifunctional separator fabricated with N-doped carbon-embedded cobalt-doped titanium nitride nanowires (NC-Ti0.95Co0.05N NWs) under 1 vol% DMA electrolyte achieved a discharge capacity of 464.4 mA h g−1 even after 200 cycles at a decay rate of 0.093% per cycle through the synergistic effects of electrolyte and electrocatalyst modifications. This work highlights the importance of ferromagnetic catalysts with a high donor-number solvent for lithium–sulfur (Li–S) batteries.
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