Dong Huiyi, Wang Lu, Cheng Yi, Sun Huiyue, You Tianqi, Qie Jingjing, Li Yifan, Hua Wuxing, Chen Ke
Center for the Physics of Low-Dimensional Materials, Henan Joint International Research Laboratory of New Energy Materials and Devices, School of Physics and Electronics, Henan University, Kaifeng, 475004, China.
School of Materials Science and Engineering, Shandong University, Jinan, 250061, China.
Adv Sci (Weinh). 2024 Sep;11(35):e2405351. doi: 10.1002/advs.202405351. Epub 2024 Jul 16.
The "shuttle effect" issue severely hinders the practical application of lithium-sulfur (Li-S) batteries, which is primarily caused by the significant accumulation of lithium polysulfides in the electrolyte. Designing effective catalysts is highly desired for enhancing polysulfide conversion to address the above issue. Here, the one-step flash-Joule-heating route is employed to synthesize a W-WC heterostructure on the graphene substrate (W-WC/G) as a catalytic interlayer for this purpose. Theoretical calculations reveal that the work function difference between W (5.08 eV) and WC (6.31 eV) induces an internal electric field at the heterostructure interface, accelerating the movement of electrons and ions, thus promoting the sulfur reduction reaction (SRR) process. The high catalytic activity is also confirmed by the reduced activation energy and suppressed polysulfide shuttling by in situ Raman analyses. With the W-WC/G interlayer, the Li-S batteries exhibit an outstanding rate performance (665 mAh g at 5.0 C) and cycle steadily with a low decay rate of 0.06% over 1000 cycles at a high rate of 3.0 C. Moreover, a high areal capacity of 10.9 mAh cm (1381.4 mAh g) is obtained with a high area sulfur loading of 7.9 mg cm but a low electrolyte/sulfur ratio of 9.0 µL mg.
“穿梭效应”问题严重阻碍了锂硫(Li-S)电池的实际应用,这主要是由多硫化锂在电解液中的大量积累所致。为解决上述问题,迫切需要设计有效的催化剂来促进多硫化物的转化。在此,采用一步闪速焦耳加热路线在石墨烯基底上合成了W-WC异质结构(W-WC/G)作为催化中间层。理论计算表明,W(5.08 eV)和WC(6.31 eV)之间的功函数差在异质结构界面处诱导出内电场,加速了电子和离子的移动,从而促进了硫还原反应(SRR)过程。原位拉曼分析通过降低活化能和抑制多硫化物穿梭也证实了其高催化活性。有了W-WC/G中间层,Li-S电池展现出出色的倍率性能(在5.0 C时为665 mAh g),并在3.0 C的高倍率下稳定循环1000次,衰减率低至0.06%。此外,在硫负载量高达7.9 mg cm但电解液/硫比低至9.0 µL mg的情况下,获得了10.9 mAh cm(1381.4 mAh g)的高面积容量。