journal article·2025-01Open access

Regulating the Local Spin States in Spinel Oxides to Promote the Activity of Li‐CO2 Batteries

Yingqi Liu, Xinru Wu, Haotian Qu, Gongxun Lu, Yanli Chen, Bingyi Lu, Yanze Song, Guangmin Zhou, Hui‐Ming Cheng

Advanced Materials· Volume 37· Issue 1

Abstract

Abstract Due to the high energy barrier, slow reaction kinetics, and complex reaction environments of Li‐CO2 batteries, the development of durable and efficient catalysts is essential. Transition metal oxides are promising for their availability, stability, and 3d electronic features, with spin states playing an important role in CO2 activation. In this study, the local spin states are regulated by incorporating Ni into Co3O4 and its impact on activity in Li‐CO2 batteries is explored. The results show that Ni atoms with high spin states in Ni0.1Co2.9O4 facilitate electron transfer from the catalyst to the unoccupied orbitals of CO2, providing sufficient active sites for the nucleation and growth of small Li2CO3 crystals. These small crystals have a low decomposition barrier, leading to improved battery efficiency. Therefore, Ni0.1Co2.9O4 shows superior catalytic performance with an overpotential of 0.72 V and an energy efficiency of ≈70% after 500 h. This work provides insights into the relationship between spin states and CO2 reactions, highlighting a promising avenue for developing high‐performance metal‐CO2 batteries.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Inorganic Chemistry and Materials

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

Affiliations

Tsinghua‐Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

College of Physics Guizhou University Guiyang 550025 China

Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Shenyang 110016 China

Shenzhen Key Lab of Energy Materials for Carbon Neutrality Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China

Faculty of Materials Science and Energy Engineering Shenzhen University of Advanced Technology Shenzhen 518055 China

Funding

National Natural Science Foundation of China · Guangdong Innovative and Entrepreneurial Research Team Program · China Postdoctoral Science Foundation · Shenzhen Science and Technology Innovation Program

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