Citation: Ye Yaokun, Hu Zongxiang, Liu Jiahua, Lin Weicheng, Chen Taowen, Zheng Jiaxin, Pan Feng. Research Progress of Theoretical Studies on Polarons in Cathode Materials of Lithium-Ion Batteries[J]. Acta Physico-Chimica Sinica, ;2021, 37(11): 201100. doi: 10.3866/PKU.WHXB202011003 shu

Research Progress of Theoretical Studies on Polarons in Cathode Materials of Lithium-Ion Batteries

School of Advanced Materials, Peking University, Shenzhen Graduate School, Shenzhen 518055, Guangdong Province, China

Corresponding author: Zheng Jiaxin, zhengjx@pkusz.edu.cn Pan Feng, panfeng@pkusz.edu.cn

^†

Received Date: 2 November 2020
Revised Date: 10 December 2020
Accepted Date: 10 December 2020
Available Online: 16 December 2020
Fund Project: the Shenzhen Science and Technology Innovation Committee ZDSYS20170728102618the National Natural Science Foundation of China 21603007The project was supported by the National Key R&D Program of China (2016YFB0700600), the National Natural Science Foundation of China (21603007, 51672012), the Guangdong Key-lab Project (2017B0303010130), and the Shenzhen Science and Technology Innovation Committee (ZDSYS20170728102618)the National Natural Science Foundation of China 51672012the Guangdong Key-lab Project 2017B0303010130the National Key R&D Program of China 2016YFB0700600

In addition to their extensive commercial application in electronic devices such as cell phones and laptops, lithium-ion batteries (LIBs) are most suitable to fulfill the energy storage requirements of electric vehicles because of their recognized safety, portability, and high energy density. Cathodes are the most important part of LIBs, and various cathode materials have been widely investigated over the past decades. Polaron formation has been attracting increasing attention in the research of cathode materials, as it limits electron conduction. In particular, polarons are responsible for low electronic conductivity in cathode materials like olivine phosphate. Polaron is a typical crystal defect caused by the integrated motion of lattice distortion and its trapping electrons. Research on the mechanism of polaron formation will provide theoretical guidance for the design of high-electronic-conductivity cathode materials and improvement of the electrochemical performance of LIBs. Theoretical calculation is a direct and important method to study polaron formation in a specific crystal material, because the presence of polarons and their formation mechanisms can be effectively verified through this method. In this article, we first introduce the basic physical concept of polarons and their dynamical model according to the Marcus and Emin-Holstein-Austin-Mott theories. A comparison of the general properties of large and small polarons, summarized in this chapter, reveals that small polaron formation more likely occurs in cathode materials. Moreover, the theoretical characterization, electrical impact, control and challenges of polarons are reviewed. Although a universal necessary and suitable condition for the theoretical characterization of polarons has not yet been found, we still propose three criteria that are proven to be feasible and practical for the theoretical identification of polarons when applied in combination. Experimental characterizations are also introduced briefly for reference, because the comparison with the experiment is suggested to be necessary and mandatory. The electrical impact caused by polarons results in low electronic conductivity, which has been broadly reported in layered, olivine, and spinel cathode materials. Doping can weaken the influence of polarons and, thus, significantly enhance the electronic conductivity, thereby becoming the most prevalent strategy for tuning polarons. Although theoretical calculations have been widely and effectively conducted in the study of polarons, some challenges may still be faced because of the intrinsic shortcomings of the traditional density functional theory, which need to be addressed. Finally, further research on polarons from the perspective of basic theory and practical applications is prospected.
- Polaron,
- Lithium-ion battery,
- Cathode materials,
- Electronic conductivity,
- First-principle calculations
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