Intrinsic stabilization of vacancies in catalysts via high-entropy approach for lithium-sulfur batteries

利用高熵方法实现锂硫电池催化剂中空位的本征稳定化

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Abstract

Oxygen vacancies (V(O)) have been considered as a significant strategy to improve the performance of catalysts in Li-S batteries. However, the highly active V(O) are a double-edged sword, as their instability can undermine long-term cycle performance. Therefore, it is essential to stabilize V(O) while maintaining their high activity. Here, five different metal elements are dissolved into the lattice structure of two-dimensional oxides to construct intrinsically stable and active V(O) for better lithium-sulfur catalysts. The unique electronic and crystal structure in high-entropy oxide endows the changed differentiated formation energies and high diffusion energy barrier of V(O) to form intrinsically stable V(O). The Li-S batteries with stable V(O) in the electrocatalyst deliver a high specific capacity of 1301 mAh g(-1) at 0.2C and low capacity fading of 0.032% per cycle after 2000 cycles at 1C. This work will inspire efforts on breaking the trade-off between activity and stability in heterogeneous catalysis beyond Li-S batteries.

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