题目: | stabilized oxygen vacancy chemistry toward high-performance layered oxide cathodes for sodium-ion batteries |
作者: | chen cheng1#, zengqing zhuo2#, xiao xia1#, tong liu3, yihao shen1, cheng yuan1, pan zeng4, duanyun cao3,5, ying zou6, jinghua guo2, and liang zhang1* |
单位: | 1institute of functional nano & soft materials (funsom),jiangsu key laboratory of advanced negative carbon technologies, soochow university, suzhou 215123, china 2advanced light source, lawrence berkeley national laboratory, berkeley, california 94720, united states 3beijing key laboratory of environmental science and engineering, school of materials science and engineering, beijing institute of technology, beijing 100081, china 4institute for advanced study, school of mechanical engineering, chengdu university, chengdu 610106, china 5chongqing innovation center, beijing institute of technology, chongqing 401120, china 6shanghai synchrotron radiation facility, shanghai advanced research institute, chinese academy of sciences, shanghai 201204, china |
摘要: | anionic redox has emerged as a transformative paradigm for high-energy layered transition-metal (tm) oxide cathodes, but it is usually accompanied by the formation of anionic redox-mediated oxygen vacancies (ovs) due to irreversible oxygen release. additionally, external factor-induced ovs (defined as intrinsic ovs) also play a pivotal role in the physicochemical properties of layered tm oxides. however, an in-depth understanding of the interplay between intrinsic and anionic redox-mediated ovs and the corresponding regulation mechanism of the dynamic evolution of ovs is still missing. herein, we disclose the strong interrelationship between these ovs and demonstrate that the presence of intrinsic ovs in the tmo2 layers could induce weak integrity of the tm-o frameworks and unlock additional diffusion paths to trigger the generation and migration of anionic redox-mediated ovs. accordingly, an ov stabilization strategy is proposed by deliberately introducing high-valence nb5 , which could serve as an important building block in anchoring the oxygen sublattice and preventing the formation of a percolating ov migration network, thereby suppressing the formation/diffusion of anionic redox-mediated ovs. consequently, superb structural integrity and improved electrochemical performance with reversible anionic redox chemistry are achieved. this work advances our understanding of the role of ovs for developing high-performance energy storage systems utilizing anionic redox. |
影响因子: | 15.8 |
分区情况: | 一区 |
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