Jung Roland, Metzger Michael, Maglia Filippo, Stinner Christoph, Gasteiger Hubert A
Chair of Technical Electrochemistry, Department of Chemistry and Catalysis Research Center, Technische Universität München , Lichtenbergstrasse 4, 85748 Garching, Germany.
BMW AG , Petuelring 130, 80788 Munich, Germany.
J Phys Chem Lett. 2017 Oct 5;8(19):4820-4825. doi: 10.1021/acs.jpclett.7b01927. Epub 2017 Sep 21.
We compare the stability of alkyl carbonate electrolyte on NMC111, -622, and -811, LNMO, and conductive carbon electrodes. We prove that CO and CO evolution onset potentials depend on the electrode material and increase in the order NMC811 < NMC111 ≈ NMC622 < conductive carbon ≈ LNMO, which we rationalize by two fundamentally different oxidation mechanisms, the chemical and the electrochemical electrolyte oxidation. Additionally, in contrast to the widespread understanding that transition metals in cathode active materials catalyze the electrolyte oxidation, we will prove that such a catalytic effect on the electrochemical electrolyte oxidation does not exist.
我们比较了碳酸烷基酯电解质在NMC111、-622、-811、LNMO和导电碳电极上的稳定性。我们证明,CO和CO析出起始电位取决于电极材料,且按照NMC811 < NMC111 ≈ NMC622 < 导电碳 ≈ LNMO的顺序增加,我们通过两种根本不同的氧化机制,即化学和电化学电解质氧化来解释这一现象。此外,与广泛认为的阴极活性材料中的过渡金属催化电解质氧化的观点相反,我们将证明这种对电化学电解质氧化不存在催化作用。