Experimental Investigation and First-Principles Calculations of a Ni3Se4 Cathode Material for Mg-Ion Batteries

Luyao Wei; Ruqian Lian; Yingying Zhao; Yuan Meng; Li He; Yue Yu; Gang Chen; Yingjin Wei

doi:10.1021/acsami.9b21540

Experimental Investigation and First-Principles Calculations of a Ni₃Se₄ Cathode Material for Mg-Ion Batteries

ACS Appl Mater Interfaces. 2020 Feb 26;12(8):9316-9321. doi: 10.1021/acsami.9b21540. Epub 2020 Feb 17.

Authors

Luyao Wei¹, Ruqian Lian¹, Yingying Zhao², Yuan Meng³, Li He¹, Yue Yu¹, Gang Chen¹, Yingjin Wei¹

Affiliations

¹ Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education), Jilin Engineering Laboratory of New Energy Materials and Technology, College of Physics , Jilin University , Changchun 130012 , P.R. China.
² College of Physics and Optoelectronic Engineering , Harbin Engineering University , Harbin 150001 , China.
³ School of Materials Science and Engineering , Changchun University of Science and Technology , Changchun 130022 , China.

PMID: 32028767
DOI: 10.1021/acsami.9b21540

Abstract

Magnesium ion batteries (MIBs) have attracted increasing attention due to their advantages of abundant reserves, low price, and high volumetric capacity. However, the large Coulombic interactions of Mg²⁺ with the cathode framework seriously hinder the rate capability and cycle stability of the battery cell. For this reason, finding a suitable cathode material has become a main task in MIB research. In this study, Ni₃Se₄ was first proposed as a new cathode material for MIBs. First-principles calculations showed that Ni₃Se₄ could accommodate up to 1 mol of Mg²⁺, but the migration energy barrier was as high as 1.35 eV. Accordingly, nanosized Ni₃Se₄ was prepared by a hydrothermal method to achieve satisfying electrochemical performance. The prepared Ni₃Se₄ material showed a discharge capacity of 99.8 mA·h·g^-1 at 50 mA·g^-1 current density with a capacity retention of 75% after 100 cycles. Combined with first-principles calculations and spectroscopic studies, it was demonstrated that the material underwent a solid-solution structural change during Mg²⁺ insertion, with all charge transfer taking place on the Ni cations.

Keywords: Mg-ion batteries; Ni3Se4; cathode material; electrochemical properties; first-principles calculations.