Adv. Funct. Mater.: Chemomechanics Engineering Promotes the Catalytic Activity of Spinel Oxides for Sulfur Redox Reaction

Title：

Chemomechanics Engineering Promotes the Catalytic Activity of Spinel Oxides for Sulfur Redox Reaction

Authors：

Lei Wang^1,2, Hongtai Li^1,2, Tianran Yan^1,2, Cheng Yuan^1,2, Genlin Liu^1,2, Gang Zhao^1,2, Pan Zeng³, and Liang Zhang^1,2*

Institutions：

¹Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China

²Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, 215123, China

³Institute for Advanced Study School of Mechanical Engineering, Chengdu University, Chengdu 610106, China

Abstract：

Cooperative catalysis is a promising approach to enhance the sluggish redox kinetics of lithium polysulfides (LiPSs) for practical lithium–sulfur (Li–S) batteries. However, the elusory synergistic effect among multiple active sites makes it challenging to accurately customize the electronic structure of catalysts. Herein, a strategy of precisely tailoringe_gorbitals of spinel oxides through chemomechanics engineering is porposed to regulate LiPSs retention and catalysis. By manipulating the regulable cations in Mn_xCo_3-xO₄, it is theoretically and experimentally revealed that the lattice strain induced by the Jahn–Teller active and high-spin Mn³⁺at octahedral (Oh) sites can increase thee_goccupancy of low-spin Co³⁺_Oh, which effectively regulates the chemical affinity toward LiPSs and establishes an unblocked channel for intrinsic charge transfer. This leads to a volcano-type correlation between thee_goccupancy at Oh sites and sulfur redox activity. Benefitting from the cooperative catalysis of dual-active sites, MnCo₂O₄with an averagee_goccupancy of 0.45 affords the most appropriate adsorption strength and rapid redox kinetics toward LiPSs, leading to remarkable rate performance and capacity retention for the assembled Li–S batteries. This work demonstrates the promise of chemomechanics engineering for optimizing thee_goccupancy to achieve efficient sulfur redox catalysts.

IF：

19.00

Link：

https://onlinelibrary.wiley.com/doi/10.1002/adfm.202404184