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Improving the rate capability of high voltage Lithium-ion battery cathode material LiNi0.5Mn1.5O4 by ruthenium doping

: Kiziltaş-Yavuz, Nilüfer; Bhaskar, Aiswarya; Dixon, Ditty; Yavuz, Murat; Nikolowski, Kristian; Lu, Li; Eichel, Rüdiger; Ehrenberg, Helmut


Journal of power sources 267 (2014), S.533-541
ISSN: 0378-7753
Fraunhofer IKTS ()
high-voltage cathode; lithium ion batteries; ruthenium doping; spinel

The citric acid-assisted sol–gel method was used to produce the high-voltage cathodes LiNi0.5Mn1.5O4 and LiNi0.4Ru0.05Mn1.5O4 at 800 °C and 1000 °C final calcination temperatures. High resolution powder diffraction using synchrotron radiation, inductively coupled plasma – optical emission spectroscopy and scanning electron microscopy analyses were carried out to characterize the structure, chemical composition and morphology. X-ray absorption spectroscopy studies were conducted to confirm Ru doping inside the spinel as well as to compare the oxidation states of transition metals. The formation of an impurity LixNi1−xO in LiNi0.5Mn1.5O4 powders annealed at high temperatures (T ≥ 800 °C) can be suppressed by partial substitution of Ni2+ by Ru4+ ion. The LiNi0.4Ru0.05Mn1.5O4 powder synthesized at 1000 °C shows the highest performance regarding the rate capability and cycling stability. It has an initial capacity of ∼139 mAh g−1 and capacity retention of 84% after 300 cycles at C/2 charging–discharging rate between 3.5 and 5.0 V. The achievable discharge capacity at 20 C for a charging rate of C/2 is ∼136 mAh g−1 (∼98% of the capacity delivered at C/2). Since the electrode preparation plays a crucial role on parameters like the rate capability, the influence of the mass loading of active materials in the cathode mixture is discussed.