多支化氮化钒电催化剂实现锂硫电池的宽温运行,ACS Nano

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多支化氮化钒电催化剂实现锂硫电池的宽温运行
ACS Nano ( IF 15.8 ) Pub Date : 2023-06-08 , DOI: 10.1021/acsnano.3c01469
Lianbo Ma _{1,

2} , Yanrong Wang _{2,

3} , Ziwei Wang ₁ , Junling Wang ₄ , Yuwen Cheng ₁ , Junxiong Wu ₅ , Bo Peng ₁ , Jie Xu ₁ , Wei Zhang ₄ , Zhong Jin ₂

Affiliation

能够在恶劣条件下正常工作的高性能锂硫（Li-S）电池引起了极大的关注；然而，低温下多硫化物转化反应动力学缓慢以及高温下多硫化物穿梭问题仍有待解决。在此，我们设计并部署了一种用于锂硫电池的多支化氮化钒（MB-VN）电催化剂。实验（飞行时间二次离子质谱和吸附测试）和理论结果都验证了MB-VN对多硫化物的强化学吸附能力和高电催化活性。此外，原位拉曼表征表明MB-VN电催化剂可以有效抑制多硫化物穿梭。使用 MB-VN 改进的分隔符，^–1在 3.0 C 下）和室温下出色的循环稳定性（在 1.0 C 下 400 次循环后为 678 mAh g ^{–1 ）。}硫含量为 6.0 mg cm ^–2，贫电解液体积为 ∼6 µL mg _s^{–1 ，Li-S 电池表现出 5.47 mAh cm}^–2的高面积容量。即使在很宽的温度范围（−20至+60°C）下，锂硫电池仍然在高电流倍率下保持稳定的循环性能。这项工作表明，基于金属氮化物的电催化剂可以实现耐低温/高温的锂硫电池。

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Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

High-performance lithium–sulfur (Li–S) batteries that can work normally under harsh conditions have attracted tremendous attention; however, the sluggish reaction kinetics of polysulfide conversions at low temperatures as well as the notorious polysulfide shuttling at high temperatures remain to be resolved. Herein, a multibranched vanadium nitride (MB-VN) electrocatalyst has been designed and deployed for Li–S batteries. Both experimental (time-of-flight secondary ion mass spectroscopy and adsorption tests) and theoretical results verify the strong chemical adsorption capability and high electrocatalytic activity of MB-VN with respect to polysulfides. Moreover, in situ Raman characterization manifests the effective inhibition of polysulfide shuttling by the MB-VN electrocatalyst. Using MB-VN-modified separators, the Li–S batteries deliver an excellent rate capability (707 mAh g^–1 at 3.0 C) and great cyclic stability (678 mAh g^–1 after 400 cycles at 1.0 C) at room temperature. With 6.0 mg cm^–2 of sulfur and a lean electrolyte volume of ∼6 μL mg_s^–1, Li–S batteries exhibit a high areal capacity of 5.47 mAh cm^–2. Even over a wide temperature range (−20 to +60 °C), the Li–S batteries still maintain stable cyclic performance at high current rates. This work demonstrates that metal nitride based electrocatalysts can realize low-/high-temperature-tolerant Li–S batteries.

更新日期：2023-06-08

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