Three different structures of the composition Li2Ni2TeO6 have been synthesized and their electrochemical properties characterized: a disordered orthorhombic phase with tellurium ordering and strong Li/Ni cation mixing, a T#2-layered phase, and an O3-layered phase; each have a distinct cycling performance. The disordered orthorhombic structure is the most stable at room temperature and has the highest capacity with the lowest overpotential. The T#2 phase is the least stable and undergoes a phase transformation once lithium is extracted. Density functional theory calculations reconcile the relative structural stabilities and physical properties of each phase with their electrochemical performances. Calculations also confirmed experimental observations regarding the synthesis of each structure and indicated the mechanism for capacity fade of each Li2Ni2TeO6 cathode. Strong tellurium-oxygen covalent bonding increases the voltage of the Ni2+/3+ redox couple in each of these materials over what is normally observed in layered oxides.
Bibliographical noteFunding Information:
G.H. and J.B.G. would like to acknowledge the support of the Robert A. Welch Foundation, Houston, Texas (Grant Nos. F-1066 and F-1841). N.S.G. would like to acknowledge financial support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0005397. Computational resources were provided by the Texas Advanced Computing Center and the National Energy Research Scientific Computing Center. The authors would like to acknowledge the X-ray diffraction facilities within the Texas Materials Institute.
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