Volume 9 Issue 5
May  2024
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Article Navigation >  Green Energy&Environment  > 2024  >  9(5): 909-918
Peng Gao, Pei Tang, Ying Mo, Peitao Xiao, Wang Zhou, Shi Chen, Hongliang Dong, Ziwei Li, Chaohe Xu, Jilei Liu. Covalency competition induced selective bond breakage and surface reconstruction in manganese cobaltite towards enhanced electrochemical charge storage. Green Energy&Environment, 2024, 9(5): 909-918. doi: 10.1016/j.gee.2022.10.003
Citation: Peng Gao, Pei Tang, Ying Mo, Peitao Xiao, Wang Zhou, Shi Chen, Hongliang Dong, Ziwei Li, Chaohe Xu, Jilei Liu. Covalency competition induced selective bond breakage and surface reconstruction in manganese cobaltite towards enhanced electrochemical charge storage. Green Energy&Environment, 2024, 9(5): 909-918. doi: 10.1016/j.gee.2022.10.003
shu

Covalency competition induced selective bond breakage and surface reconstruction in manganese cobaltite towards enhanced electrochemical charge storage

doi: 10.1016/j.gee.2022.10.003

  • a. College of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha, Hunan, 410082, China;

  • b. Department of Materials Science and Engineering, National University of Defense Technology, Changsha, Hunan, 410073, China;

  • c. Joint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macau, 999078, China;

  • d. Center for High Pressure Science and Technology Advanced Research, Pudong, Shanghai, 201203, China;

  • e. College of Aerospace Engineering, Chongqing University, Chongqing, 400044, China

Funds:

This work was financially supported by the National Key Research and Development Program of China (2022YFE0206300), the National Natural Science Foundation of China (22209047, U21A2081, 22075074), Natural Science Foundation of Hunan Province (2020JJ5035), Hunan Provincial Department of Education Outstanding Youth Project (23B0037), and Macau Science and Technology Development Fund (Macau SAR, FDCT-0096/2020/A2).

  • Received date 22 July 2022, Accepted date 12 October 2022, RevRecd date 30 September 2022, Publish date 29 October 2022,
    Abstract
  • Manganese cobaltite (MnCo2O4) is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability. Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into δ-MnO2 nanosheets irreversibly, thus results in a change of the reaction mechanism with K+ ion intercalation. However, the low capacity has greatly limited its practical application. Herein, we found that the tetrahedrally-coordinated Co2+ ions were leached when MnCo2O4 was equilibrated in 1 mol L-1 HCl solution, leading to the formation of layered CoOOH on MnCo2O4 surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free CoO6 octahedra. The as-formed CoOOH is stable upon cycling in alkaline electrolyte, exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution, thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion. In general, our work not only offers a feasible approach to deliberate modification of MnCo2O4's surface structure, but also provides an in-depth understanding of its charge storage mechanism, which enables rational design of the spinel oxides with promising charge storage properties.

     

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