Lithium-ion cells produce a considerable amount of gas in their first cycle. If the gases are not removed in a degassing step, most are consumed by the cell over time. This phenomenon has never been investigated explicitly in the literature. In this paper, the evolution and subsequent consumption of gas in typical lithium-ion cells are measured by Archimedes' principle and gas chromatography. It is found that all evolved gases are subsequently consumed to some degree, except for saturated hydrocarbons. The consumption of gas occurs predominantly at the negative electrode, where the gases are reduced to form part of the solid-electrolyte interphase (SEI). Changes to the negative electrode SEI upon gas consumption are investigated using X-ray photoelectron spectroscopy. The effect of gas consumption on cell performance is studied with ultra-high precision charging and high voltage storage experiments. It is found that gas consumption does not result in measurable adverse effects to cell performance. Lithium-ion cells can produce a significant amount of gas during the first charge (in the formation cycle), as electrolyte and additives react at the surfaces of the charging electrodes to form passivating films. If lithium-ion cells are packaged in a flexible casing, these gases are normally removed by the manufacturer in a degassing step, to prevent deformation of the cell and to ensure uniform stack pressure on the electrodes. If the degassing step is omitted, a large portion of the gas evolved is consumed over time.1 The reactions that consume gas are presumably prevalent in hard-cased cylindrical cells, such as 18650 s, which are often hermetically sealed before the first charge, and therefore cannot be easily degassed. The reactions that consume gas are presumably less prevalent in pouch-type cells, which are degassed.Several authors have speculated about the fates of gases in lithiumion cells.2-5 There has been no work explicitly dedicated to understanding the phenomenon of gas consumption. There is no consensus as to whether the effects of gas consumption are beneficial or harmful to cell performance. For example, it has been argued by some that the consumption of CO 2 is beneficial to cells, as it reacts to form a passivating film on the negative electrode. 3,4,6 However it has also been argued that the consumption of CO 2 is detrimental to cells, as it may reduce at the negative electrode to form Li 2 C 2 O 4 , which causes continual self-discharge at high voltage. 2It is important for both scientists and manufacturers of lithium-ion cells to understand the causes and the effects of gas consumption. If gas consumption is quick, benign, or even beneficial to cell performance, then the time-consuming degassing step for lithium-ion pouch cells might be skipped. 7 The gases evolved in lithium-ion pouch cells could be left for consumption within the cell, perhaps leaving the pouch cell flat and rigid after several hours if all the gases were consumed. If gas consumption in a cell produces undesirable effects, such...
A set of LiNi 0.5 Mn 0.3 Co 0.2 O 2 /graphite lithium-ion cells underwent 750 charge-discharge cycles during about 8 months at 55 • C to upper cutoff potentials of 4.0, 4.1, 4.2, 4.3, and 4.4 V. The electrolyte in these cells was extracted using a centrifuge method and studied using gas chromatography/mass spectrometry to determine the changes to the solvents and by inductively coupled plasma-mass spectrometry to determine the changes to the salt content in the electrolyte. The negative electrodes from the cells were harvested and studied by micro-X-ray fluorescence to quantify the amount of transition metals which migrated from the positive electrode to the negative electrode during the testing. Emphasis is given to a detailed description of the quantitative methods used in the hope that others will adopt them in similar studies of different types of aged lithium-ion cells. The cells studied here initially had 1.1 molal LiPF 6 ethylene carbonate (EC): ethyl methyl carbonate (EMC) (3:7 by weight) electrolyte. The aged cells showed increasing amounts of dimethyl carbonate and diethyl carbonate created by transesterification as the upper cutoff potential increased. Only extremely small amounts of Mn, less than 0.1% of the total Mn in the positive electrode, were found on the negative electrode after this aggressive testing. Lithium-ion batteries are currently used in a wide range of applications: cell phones, power tools, vehicles and even grid energy storage.
Small, organic‐rich lakes are important sources of methane (CH4) and carbon dioxide (CO2) to the atmosphere, yet the sensitivity of emissions to climate warming is poorly constrained and potentially influenced by permafrost thaw. Here, we monitored emissions from 20 peatland lakes across a 1,600 km permafrost transect in boreal western Canada. Contrary to expectations, we observed a shift from source to sink of CO2 for lakes warmer regions, driven by greater primary productivity associated with greater hydrological connectivity to lakes and nutrient availability in the absence of permafrost. Conversely, an 8‐fold increase in CH4 emissions in warmer regions was associated with water temperature and shifts in microbial communities and dominant anaerobic processes. Our results suggest that the net radiative forcing from altered greenhouse gas emissions of northern peatland lakes this century will be dominated by increasing CH4 emissions and only partially offset by reduced CO2 emissions.
Many studies of Li-ion cells examine compositional changes to electrolyte and electrodes to determine desirable or undesirable reactions that affect cell performance. Cells involved in these studies typically have a limited test lifetime due to the resource intensive and time-consuming nature of these experiments. Here, electrolyte and electrode analyses were performed on a large matrix of cells tested at various conditions and with various cycle lifetimes. The matrix included LiNi0.5Mn0.3Co0.2O2 (NMC532)/graphite and LiNi0.6Mn0.2Co0.2O2 (NMC622)/graphite pouch cells with excellent performing electrolyte mixtures, both cycling and storage protocols at 40 °C and 55 °C with both 4.3 V and 4.4 V upper cutoff potentials. This study presents post-test analysis (electrochemical impedance spectroscopy, differential voltage analysis, differential thermal analysis), electrolyte analysis (gas chromatography, quantitative nuclear magnetic resonance), and electrode analysis (micro X-ray fluorescence) for these cells after 3, 6, 9, and 12 months of testing. Many products and reactants, such as fraction of transesterification, gas production, transition metal dissolution appeared to have a constant rate of increase in this 12-month observation period. In most cases, results from cells after 3 to 6 months of testing could be used to reasonably estimate the status of the cells (electrolyte composition, gas production, transition metal dissolution) at 12 months.
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