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Tuning functional two-dimensional MXene nanosheets to enable efficient sulfur utilization in lithium-sulfur batteries
Cell Reports Physical Science ( IF 7.9 ) Pub Date : 2021-06-29 , DOI: 10.1016/j.xcrp.2021.100480
Rahul Pai , Varun Natu , Maxim Sokol , Michael Carey , Michel W. Barsoum , Vibha Kalra

Practicality of lithium-sulfur batteries is severely hindered by the notorious polysulfide-shuttle phenomenon, leading to rapid capacity fade. This issue is aggravated with increase in sulfur loading, causing low-coulombic efficiency and cycle life. Herein, we present a facile strategy to combine hydrophobic sulfur and hydrophilic, conductive Ti3C2Tz-MXene via one-step surface functionalization using di(hydrogenated tallow)benzylmethyl ammonium chloride (DHT). The latter renders the Ti3C2Tz surface hydrophobic, making it readily dispersible in sulfur dissolved in a carbon disulfide (CS2) solvent. By evaporating the solvent, we conformally coat the DHT-Ti3C2Tz (DMX) with sulfur. The developed composite, with higher available active area, enables effective trapping of lithium polysulfides (LiPs) on the electroactive sites within the cathode, leading to improvement in electrochemical performance at higher sulfur loadings. The DMX/S cathodes function with high sulfur loading of ∼10.7 mg·cm−2 and deliver a stable areal capacity of ∼7 mAh·cm−2 for 150 cycles. Moreover, a DMX/S cathode in a pouch-cell configuration retains ∼770 mAh·g−1 after ∼200 cycles at 0.2C (85.5% retention). Ex situ studies elucidate the nature of the LiPs-MXene interaction and the effect of surface functionalization towards improved performance.



中文翻译:

调整功能性二维 MXene 纳米片以实现锂硫电池中硫的高效利用

臭名昭著的多硫化物穿梭现象严重阻碍了锂硫电池的实用性,导致容量快速衰减。这个问题随着硫负载的增加而加剧,导致低库仑效率和循环寿命。在此,我们提出了一种使用二(氢化牛油)苄基甲基氯化铵(DHT)通过一步表面功能化将疏水性硫和亲水性导电性 Ti 3 C 2 T z -MXene结合的简便策略。后者使 Ti 3 C 2 T z表面疏水,使其易于分散在溶解在二硫化碳 (CS 2 ) 溶剂中的硫中。通过蒸发溶剂,我们共形地涂覆 DHT-Ti3 C 2 T z (DMX) 与硫。所开发的复合材料具有更高的可用活性面积,能够有效地将多硫化锂 (LiP) 捕获在阴极内的电活性位点上,从而改善更高硫负载下的电化学性能。DMX/S 正极具有~10.7 mg·cm -2 的高硫负载量,并提供~7 mAh·cm -2的稳定面积容量,循环150次。此外,软包电池配置中的 DMX/S 阴极在0.2C 下约 200 次循环后仍保持约 770 mAh·g -1(保持率为 85.5%)。易地研究阐明嘴唇,MXene相互作用的性质和表面功能化向更高的性能的影响。

更新日期:2021-07-21
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