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Published on: November 11, 2013
Heterointerface engineering via dual modification stabilizes O3-type layered oxides cathodes for high-voltage
Wei Li1, Wei Huang1, Man Zhang2
1Guangxi Key Laboratory of Low Carbon Energy Materials, Guangxi Scientific and Technological Achievements Transformation Pilot Research Base of Electrochemical Energy Materials and Devices, School of Chemistry and Pharmaceutical Sciences, Guangxi Normal University, Guilin 541004, China.
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O3-type layered sodium-based oxide cathode materials have become important candidate materials for the commercial application of sodium-ion batteries due to their high theoretical capacity. However, complex phase transitions and lattice oxygen precipitation lead to the gradual deterioration of the bulk phase structure and surface structure, resulting in the material's cycling performance fade, and becoming the main bottleneck restricting its large-scale application. Here, we designed a Sn bulk doping/SnSe2 coating modification strategy to suppress transition metal layer sliding and lattice oxygen evolution. The substitution of Ni2+ with Sn4+ not only introduces stronger SnO bonds, leading to contraction of the transition metal (TM) layers, but also generates an increased positive charge density in the TM layers due to the inequivalent doping. This results in expanded interlayer spacing between TM layers, effectively reducing electrostatic repulsion during charging and mitigating the volume changes induced by phase transformation. Meanwhile, the n-type semiconductor SnSe2 coating forms a heterostructure interface with the Sn-doped surface, effectively inhibiting the migration of oxidized oxygen anions and maintaining lattice oxygen stability under high-voltage conditions. The surface-modified O3-type layered oxide cathode exhibits significantly enhanced cycling stability, achieving a capacity retention of 71% after 500 cycles at 1C within the voltage range of 2.0-4.0 V. Even under high-voltage of 4.3 V, the material maintains 62.4% of its initial capacity after 200 cycles at 1C, which is higher than of NFM (45.6%). This study presents a SnSe2 coating/Sn-bulk doping surface modification strategy to concurrently stabilize both the bulk structure and interface of O3-type layered cathodes in sodium-ion batteries, demonstrating the potential for analogous effective strategies to be extended to other energy storage materials.
