Mo-O-C Between MoS(2) and Graphene Toward Accelerated Polysulfide Catalytic Conversion for Advanced Lithium-Sulfur Batteries.
Mo-O-C Between MoS(2) and Graphene Toward Accelerated Polysulfide Catalytic Conversion for Advanced Lithium-Sulfur Batteries.
复制标题
Mo-O-C 在 MoS 2 和石墨烯之间加速先进锂硫电池的多硫化物催化转化
DOI：
10.1002/advs.202201579
复制
发表时间：
2022-08
期刊：
影响因子：
15.1
通讯作者：
Zhou, Guangmin
中科院分区：
文献类型：
--
作者：
Zhang, Jiayu;Xu, Guobao;Zhang, Qi;Li, Xue;Yang, Yi;Yang, Liwen;Huang, Jianyu;Zhou, Guangmin
关键词：
利用范德华力构建的MoS2/C复合材料已广泛应用于锂硫（Li-S）电池。然而，由于复合界面之间的弱电子相互作用不能从根本上提高MoS2的本征电子导电性，因此对多硫化物的催化转化效果是有限的。本文通过密度泛函理论计算表明，具有Mo-O-C键的MoS2和氮掺杂碳复合材料可以促进多硫化物的催化转化，吉布斯自由能仅为0.19 eV，离解能势垒较低，为0.48 eV，这是由于在非均相界面上存在强烈的共价耦合效应。在理论计算的指导下，设计并构建了由氮掺杂还原氧化石墨烯和碳化三聚氰胺泡沫组成的坚固的二硫化钼强耦合的三维碳基体，作为锂硫电池的多功能涂层。结果，Li-S电池获得了优异的电化学性能，在5℃下的容量为615 mAh g-1，面积容量为6.11 mAh cm-2，在0.5℃下静放5天的自放电仅为8.6%。该研究为设计促进多硫化物催化转化的2D材料复合材料开辟了新的途径。密度泛函理论计算表明，具有较强共价偶联效应的MoS2/C复合材料由于具有较低的吉布斯自由能和解离能势垒，可以促进多硫化物的催化转化。随后，构建了具有Mo-O-C键的MoS2/C，具有较强的锂多硫化物化学吸附能力和丰富的催化位点，提高了锂硫电池的电化学性能。
MoS2/C composites constructed with van der Waals forces have been extensively applied in lithium–sulfur (Li–S) batteries. However, the catalytic conversion effect on polysulfides is limited because the weak electronic interactions between the composite interfaces cannot fundamentally improve the intrinsic electronic conductivity of MoS2. Herein, density functional theory calculations reveal that the MoS2 and nitrogen‐doped carbon composite with an Mo–O–C bond can promote the catalytic conversion of polysulfides with a Gibbs free energy of only 0.19 eV and a low dissociation energy barrier of 0.48 eV, owing to the strong covalent coupling effect on the heterogeneous interface. Guided by theoretical calculations, a robust MoS2 strongly coupled with a 3D carbon matrix composed of nitrogen‐doped reduced graphene oxide and carbonized melamine foam is designed and constructed as a multifunctional coating layer for lithium–sulfur batteries. As a result, excellent electrochemical performance is achieved for Li–S batteries, with a capacity of 615 mAh g–1 at 5 C, an areal capacity of 6.11 mAh cm–2, and a low self‐discharge of only 8.6% by resting for five days at 0.5 C. This study opens a new avenue for designing 2D material composites toward promoted catalytic conversion of polysulfides. Density functional theory calculations reveal that the MoS2/C composite with the strong covalent coupling effect can promote the catalytic conversion of polysulfides due to a low Gibbs free energy and dissociation energy barrier. Subsequently, MoS2/C with Mo–O–C bond is constructed and possesses strong lithium polysulfide chemical adsorption and abundant catalytic sites, enabling improved electrochemical performance of lithium–sulfur batteries.
登录
查看更多内容
MXene上离子共价有机纳米片的静电吸引和催化作用用于锂硫电池隔膜改性
影响因子：
29.4
作者：
Li, Pengyue;Lv, Haowei;Li, Xiaoju
通讯作者：
Li, Xiaoju
影响因子：
8.4
作者：
Jiang, Shouxin;Chen, Manfang;Wang, Ying
通讯作者：
Wang, Ying
影响因子：
13.3
作者：
Hu, Qianqian;Lu, Jiqun;Zhang, Lingzhi
通讯作者：
Zhang, Lingzhi
影响因子：
10.8
作者：
Li, Xia;Lushington, Andrew;Sun, Xueliang
通讯作者：
Sun, Xueliang
影响因子：
19
作者：
Balach, Juan;Jaumann, Tony;Giebeler, Lars
通讯作者：
Giebeler, Lars