Chemo‑Electrochemical Tandem Catalysis Unlocking Sulfur Reaction in Practical Lithium–Sulfur Batteries
Abstract
ABSTRACT As next‐generation high‐energy batteries, lithium–sulfur (Li–S) batteries are promising solutions for long‐range electric vehicles due to their ultrahigh theoretical energy density. However, they face fundamental challenges from low sulfur utilization, particularly under electrolyte‐starved practical conditions that polysulfides are unable to dissolve. Here, we propose a chemo‐electrochemical tandem catalyst, Li x TiS 2 , which chemically catalyzes the transformation of S 8 /Li 2 S 8 to Li 2 S 4 and subsequently catalyzes electrochemical reduction to lithium sulfide (Li 2 S). This tandem mechanism fundamentally alters the reaction kinetics from conventional first‐order to zero‐order behavior, overcoming the limitation imposed by the solubility of sulfur species. It thus enables efficient sulfur conversion and an ultralow activation energy of ∼0.3 eV (a 50% reduction compared to without catalysts) under a low electrolyte‐to‐sulfur (E/S) ratio (5 µL mg s −1 ), significantly improving battery performance in practical conditions. The coin cell shows an ultralow capacity decay of 0.028% per cycle over 1500 cycles, and a 2.0 Ah pouch cell achieves the high energy density of 550 Wh kg −1 with good stability.
Article Details
Authors (9)
Linkai Peng
Shenzhen Geim Graphene Center, Shenzhen Key Laboratory for Graphene-Based Materials, Tsinghua Shenzhen International Graduate School
Chuannan Geng
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, State Key Laboratory of Chemical Engineering and Low-Carbon Technology, School of Chemical Engineering and Technology, National Industry-Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Yaqi He
Shenzhen All‐Solid‐State Lithium Battery Electrolyte Engineering Research Center Key Laboratory of Electrocatalytic Materials and Green Hydrogen Technology of Guangdong Higher Education Institutes Shenzhen Key Laboratory for Graphene‐based Materials Institute of Materials Research Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China
Yun Cao
Key Laboratory of Evolution and Marine Biodiversity (Ministry of Education) and Institute of Evolution and Marine Biodiversity, Ocean University of China, Qingdao, China.
Jiwei Shi
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, State Key Laboratory of Chemical Engineering and Low-Carbon Technology, School of Chemical Engineering and Technology, National Industry-Education Platform for Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Jiaqi Lan
Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Key Laboratory of Electrocatalytic Materials and Green Hydrogen Technology of Guangdong Higher Education Institutes, Shenzhen Key Laboratory for Graphene-Based Materials, Institute of Materials Research, Tsinghua Shenzhen International Graduate School
Yufei Zhao
State Key Laboratory of Chemical Resource Engineering
Ziqiang Wang
Wei Lv