Abstract

Gas evolution has a profound effect on the functioning of state-of-the-art lithium-ion batteries. On one hand, it is the natural concomitant of solid electrolyte interphase (SEI) formation on the anode (reduction of electrolyte components). On the other hand, because of the demand for high terminal voltages, it is also the consequence of electrolyte and/or cathode material oxidation. Overall, gassing happens on the expense of Coulombic efficiency and additionally raises safety issues. Herein, the gassing behavior of one of the most important commercialized cathode materials, namely Ni-rich Li1 + xNi0.5Co0.2Mn0.3O2 (NCM523 with 0.01 < x < 0.05), is reported for the first time. We analyze the generation pattern of the most typical gases H2, C2H4, CO2, and CO during 30 cycles by means of differential electrochemical mass spectrometry combined with Fourier transform infrared spectroscopy. In a long-term test of an NCM523/graphite cell, we monitor its potential-resolved gas evolution and evaluate the total amount of gas from cycle to cycle. An explanation on the characteristic features of pressure versus time curves during cycling is given by combining the spectrometric and total gas pressure data. With additional information from graphite/lithium cells, the identity of gases formed during SEI formation is revealed.

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