Ultraviolet-Initiated In-Situ Cross-Linking of Multifunctional Binder Backbones Enables Robust Lithium-Sulfur Batteries

Sha Li, aState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Tan Kah Kee Innovation Laboratory, Xiamen University, Xiamen, Fujian, 361005, China
Xiao Zhana, aState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Tan Kah Kee Innovation Laboratory, Xiamen University, Xiamen, Fujian, 361005, China
Gulian Wang, bKey Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China
Huiqun Wang, aState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Tan Kah Kee Innovation Laboratory, Xiamen University, Xiamen, Fujian, 361005, China
Weiming Xiong, aState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Tan Kah Kee Innovation Laboratory, Xiamen University, Xiamen, Fujian, 361005, China
Li Zhang, aState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Tan Kah Kee Innovation Laboratory, Xiamen University, Xiamen, Fujian, 361005, China

Abstract

Lithium-sulfur (Li-S) batteries show attractive prospects owing to their high theoretical energy density, but their commercialization still faces challenges such as lithium polysulfides shuttling, severe volume change and considerable&polarization. These stubborn issues place higher demands on each component in the battery, such as the development of multifunctional binders with superior mechanical properties. Herein, ethoxylated trimethylolpropane triacrylate is firstly introduced into sulfur cathodes, in-situ cross-linked by ultraviolet (UV) curing and combined with traditional polyvinylidene difluoride binder (i.e., forming a binary binder, denoted as c-ETPTA/PVDF) to construct high-loading and durable Li-S batteries. The covalently cross-linked ETPTA framework not only significantly enhances the mechanical strength of the laminate, but also offers a strong chemical affinity for lithium polysulfides due to the abundant oxygen-containing groups. Moreover, the moderate interaction force between ether oxygen bonds and Li+ further accelerates the Li+ transport. As such, the S-c-ETPTA/PVDF electrode exhibits an ultralow attenuation rate of 0.038% at 2 C over 1000 cycles. Even under a sulfur loading of 7.8 mgS·cm-2, an average areal capacity of 6.2 mAh·cm-2 can be achieved after 50 cycles. This work indicates that light-assisted curing technology holds great promise in the fabrication of robust and high-energy-density Li-S batteries.