An Electrolyte Engineered Homonuclear Copper Complex as Homogeneous Catalyst for Lithium–Sulfur Batteries

Author:

Yang Qin1,Shen Shiying2,Han Zhiyuan3,Li Guanwu4,Liu Dong5,Zhang Qingchun1,Song Lixian1,Wang Dong4,Zhou Guangmin3ORCID,Song Yingze1ORCID

Affiliation:

1. State Key Laboratory of Environment‐Friendly Energy Materials School of Materials and Chemistry Southwest University of Science and Technology Mianyang 621010 China

2. Institute of Applied Physics and Materials Engineering University of Macau Macao SAR 999078 China

3. Tsinghua‐Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

4. Key Laboratory of Automobile Materials MOE School of Materials Science & Engineering Jilin Provincial Internation‐al Cooperation Key Laboratory of High‐Efficiency Clean Energy Materials Electron Microscopy Center and Interna‐tional Center of Future Science Jilin University Changchun 130012 China

5. Key Laboratory of Neutron Physics and Institute of Nuclear Physics and Chemistry China Academy of Engineering Physics Mianyang 621999 China

Abstract

AbstractLithium–sulfur (Li–S) batteries suffer from severe polysulfide shuttle, retarded sulfur conversion kinetics and notorious lithium dendrites, which has curtailed the discharge capacity, cycling lifespan and safety. Engineered catalysts act as a feasible strategy to synchronously manipulate the evolution behaviors of sulfur and lithium species. Herein, a chlorine bridge‐enabled binuclear copper complex (Cu‐2‐T) is in situ synthesized in electrolyte as homogeneous catalyst for rationalizing the Li–S redox reactions. The well‐designed Cu‐2‐T provides completely active sites and sufficient contact for homogeneously guiding the Li2S nucleation/decomposition reactions, and stabilizing the lithium working interface according to the synchrotron radiation X‐ray 3D nano‐computed tomography, small angle neutron scattering and COMSOL results. Moreover, Cu‐2‐T with the content of 0.25 wt% approaching saturated concentration in electrolyte further boosts the homogeneous optimization function in really operated Li–S batteries. Accordingly, the capacity retention of the Li–S battery is elevated from 51.4% to 86.3% at 0.2 C, and reaches 77.0% at 1.0 C over 400 cycles. Furthermore, the sulfur cathode with the assistance of Cu‐2‐T realizes the stable cycling under the practical scenarios of soft‐packaged pouch cell and high sulfur loading (6.5 mg cm−2 with the electrolyte usage of 4.5 µL mgS−1).

Funder

National Synchrotron Radiation Laboratory

State Key Laboratory of Environmental-friendly Energy Materials

Sichuan Province Science and Technology Support Program

Publisher

Wiley

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