journal article·2023-04

Unlock Restricted Capacity via OCe Hybridization for LiOxygen Batteries

Zhuang Sun, Xiaohui Zhao, Wujie Qiu, Bin Sun, Fan Bai, Jianjun Liu, Tao Zhang

Advanced Materials· Volume 35· Issue 14
Publisher page

Abstract

Abstract The aprotic Li‐O 2 battery (LOB) has the highest theoretical energy density of any rechargeable batteries. However, such system is largely restricted by the electrochemically formed lithium peroxide (Li 2 O 2 ) on the cathode surface, leading ultimately to low actual capacities and early cell death. In contrast to the surface‐mediated growth of thin film with a thickness <50 nm, a non‐crystalline Li 2 O 2 film with a thickness of >400 nm can be formed via an optimal OCe hybridized electronic structure. Specially, oxygen can react with dissolved cerium cations in the electrolyte via a cerium‐oxygen reaction to form a high‐energy faceted cerium oxide catalyst, which not only generates a great number of non‐saturable active sites, but also erects electron transport bridges between the lattice O and adjacent Ce atoms. Such CeO orbital hybridization also forms a direct charge transfer channel from Ce‐4f of CeO 2 to ‐π* of Li 2 O 2 , eventually leading to submicron‐thick Li 2 O 2 shells via a subsequent lithium‐oxygen reaction. Relying on the above merits, this work unlocks the rechargeable capacities of LOB from restricted 1000 to unprecedented 10 000 mAh g −1 with good cyclabilities and reduced charge–discharge overpotentials.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences 1295 Dingxi Road Shanghai 200050 P. R. China

Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China

CAS Key Laboratory of Materials for Energy Conversion Shanghai Institute of Ceramics Chinese Academy of Sciences 1295 Dingxi Road Shanghai 200050 P. R. China

Tai'an Institute of Industrial Technology Innovation‐Shandong Institutes of Industrial Technology Tai'an Branch 28 Zhengyangmen Road Taian 271000 P. R. China

Institute of BioPharmaceutical Research Liaocheng University 1 Hunan Road Liaocheng 252000 P. R. China

School of Chemistry and Materials Science Hangzhou Institute for Advanced Study University of Chinese Academy of Science 1 Sub‐lane Xiangshan Hangzhou 310024 P. R. China

Funding

National Natural Science Foundation of China · Science and Technology Commission of Shanghai Municipality · Natural Science Foundation of Shanghai · Program of Shanghai Academic Research Leader

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