Selective Adsorption and Electrocatalysis of Polysulfides through Hexatomic Nickel Clusters Embedded in N-Doped Graphene toward High-Performance Li-S Batteries
Jiapeng Ji,
Ying Sha,
Zeheng Li,
Xuehui Gao,
Teng Zhang,
Shiyu Zhou,
Tong Qiu,
Shaodong Zhou,
Liang Zhang,
Min Ling,
Yanglong Hou,
Chengdu Liang
Affiliations
Jiapeng Ji
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Ying Sha
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Zeheng Li
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Xuehui Gao
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Teng Zhang
Beijing Key Laboratory for Magnetoelectric Materials and Devices, Beijing Innovation Center for Engineering Science and Advanced Technology (BIC-ESAT), Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing 100871, China
Shiyu Zhou
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Tong Qiu
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Shaodong Zhou
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Liang Zhang
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123 Jiangsu, China
Min Ling
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
Yanglong Hou
Beijing Key Laboratory for Magnetoelectric Materials and Devices, Beijing Innovation Center for Engineering Science and Advanced Technology (BIC-ESAT), Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing 100871, China
Chengdu Liang
Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China
The shuttle effect hinders the practical application of lithium-sulfur (Li-S) batteries due to the poor affinity between a substrate and Li polysulfides (LiPSs) and the sluggish transition of soluble LiPSs to insoluble Li2S or elemental S. Here, we report that Ni hexatomic clusters embedded in a nitrogen-doped three-dimensional (3D) graphene framework (Ni-N/G) possess stronger interaction with soluble polysulfides than that with insoluble polysulfides. The synthetic electrocatalyst deployed in the sulfur cathode plays a multifunctional role: (i) selectively adsorbing the polysulfides dissolved in the electrolyte, (ii) expediting the sluggish liquid-solid phase transformations at the active sites as electrocatalysts, and (iii) accelerating the kinetics of the electrochemical reaction of multielectron sulfur, thereby inhibiting the dissolution of LiPSs. The constructed S@Ni-N/G cathode delivers an areal capacity of 9.43 mAh cm-2 at 0.1 C at S loading of 6.8 mg cm-2, and it exhibits a gravimetric capacity of 1104 mAh g-1 with a capacity fading rate of 0.045% per cycle over 50 cycles at 0.2 C at S loading of 2.0 mg cm-2. This work opens a rational approach to achieve the selective adsorption and expediting of polysulfide transition for the performance enhancement of Li-S batteries.
