Li -clipping for edge S-vacancy MoS2 quantum dots as an efficient bifunctional electrocatalyst enabling discharge growth of amorphous Li2O2 film
Li -clipping for edge S-vacancy MoS2 quantum dots as an efficient bifunctional electrocatalyst enabling discharge growth of amorphous Li2O2 film
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边缘 S 空位 MoS2 量子点的 Li 剪切作为高效双功能电催化剂，实现非晶 Li2O2 薄膜的放电生长
DOI：
10.1016/j.nanoen.2019.103996
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发表时间：
2019
期刊：
影响因子：
17.6
通讯作者：
Zhang Yue
中科院分区：
文献类型：
--
作者：
Sun Zemin;He Jinlu;Yuan Mengwei;Lin Liu;Zhang Zheng;Kang Zhuo;Liao Qingliang;Li Huifeng;Sun Genban;Yang Xiaojing;Long Run;Zhang Yue
二硫化钼（MoS2）作为一种极其有趣的具有优异电催化剂的二维（2D）材料，近年来引起了越来越多的关注。然而，缺乏精确设计的富边S空位MoS2成为深入研究氧还原反应（ORR）和析氧反应（OER）构效关系的主要障碍。在此，基于Lewis酸碱理论，我们利用双(三氟甲基磺酰)亚胺锂作为剥离剂和限幅剂，通过自上而下的策略制备了富边S空位MoS2量子点(MoS2QDs)。通过实验和理论联合研究，首次证明富边S空位MoS2QDs在Li-O2电池体系中表现出非凡的ORR/OER催化性能。重要的是，富边S空位MoS2QD可以在高电流密度下运行超过230个循环，这几乎是块状MoS2的循环稳定性的9倍。优异的活性主要是由于MoS2QDs促进了非晶Li2O2薄膜在阴极上的共形生长，这源于Li+和O2之间吸附能的显着差异，这可以显着增强Li2O2形成/分解动力学。这项工作为富边S空位MoS2QD的可控合成提供了一种新方法，建立了高OER/ORR活性的潜在机制，并提出了应用其他TMD的高可转化性。
Molybdenum disulfide (MoS2), as an extremely intriguing two-dimensional (2D) material with excellent electrocatalyst, has attracted more and more attentions in recent years. However, the lack of precisely engineered rich-edge S-vacancy MoS2constitutes a major obstacle for in-depth studying of structure-activity relationship of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, based on Lewis acid-base theory, we prepared rich-edge S-vacancy MoS2quantum dots (MoS2QDs)viatop-down strategy using lithium bis(trifluoromethylsulphonyl)imide as a stripper and clipper. It is demonstrated for the first time that the rich-edge S-vacancy MoS2QDs exhibit an extraordinary ORR/OER catalytic performance in Li-O2batteries system by a joint experimental and theoretical study. Importantly, the rich-edge S-vacancy MoS2QDs can run more than 230 cycles at high current density, which was almost 9 times longer than the cycle stability of bulk MoS2. The excellent activity arises primarily due to that the MoS2QDs facilitate conformal growth of amorphous Li2O2film on the cathode, originating from the significant differences of adsorption energies between Li+and O2, which could significantly enhanced Li2O2formation/decomposition kinetics. This work provides a novel way for controllable synthesis of rich-edge S-vacancy MoS2QDs, establishes the underlying mechanisms for the high OER/ORR activity, and suggests high translatability to apply other TMDs.