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In Situ Thermally-Driven Radial Heterophase Evolution of δ-Bi2O3 Modulates the p-Block Bi 6p Orbitals and p-Band
Shunyou Hu1, Yancen Li1, Huanchun Zhang1
1Liaoning Key Lab of Lignocellulose Chemistry and BioMaterials, Liaoning Collaborative Innovation Center for Lignocellulosic Biorefinery, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034, China.
Abstract:
The commercialization of lithium-sulfur batteries is hindered by challenges such as the shuttle effect of lithium polysulfides (LiPSs), slow sulfur redox reaction kinetics, and poor electrical conductivity. The electronic configuration of the p-block Bi 6p orbitals is modulated through an in situ thermally-induced reduction strategy using lignin-based carbon nanofibers (CNFs). This approach enables the radial gradient heterophase transformation of δ-Bi2O3, leading to the formation of a high-density heterojunction network composite (δ-Bi2O3-OVS/Bi@CNFs) rich in oxygen vacancies (OVS), which effectively moderates the adsorption of LiPSs and enhances the kinetics of sulfur redox reactions. Based on the δ-Bi2O3-OVS/Bi@CNFs, a high-energy-density (377 Wh kg-1) pouch cell with a capacity of 1.8 Ah is fabricated and successfully used in drone flights, highlighting its potential for practical applications. This work elucidates the mechanism of in situ thermally-induced radial-gradient heterophase evolution of p-block metal oxides and the influence of 6p-orbital electron modulation on the sulfur redox reaction.
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