Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights

Gauthier, Magali; Carney, Thomas J.; Grimaud, Alexis; Giordano, Livia; Pour, Nir; Chang, Hung-Ju; Fenning, David P.; Lux, Simon Franz; Paschos, Odysseas; Bauer, Christoph; Maglia, Filippo; Lupart, Saskia; Lamp, Peter; Shao‐Horn, Yang

doi:10.1021/acs.jpclett.5b01727

Cited by 878 publications

(933 citation statements)

References 235 publications

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“…The SEI acts as a protective layer to impede continuous electrolyte decomposition and solvent co-intercalation into graphitic layers during subsequent cycles. 24,25 The large charge capacity and low coulombic efficiency in the first formation cycle seen here is directly associated mainly with anode SEI formation as well as irreversible capacity loss on the cathode ( Figure S2). For example, the NMC811/SLC 1520T cell delivered a charge and discharge capacity of 224 mAh/g NMC and 192 mAh/g NMC , respectively, yielding a coulombic efficiency (CE) of 86.1% for the first formation cycle.…”

Section: Resultsmentioning

confidence: 92%

Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries

Mao

Wood

David

et al. 2018

J. Electrochem. Soc.

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Most lithium-ion batteries still rely on intercalation-type graphite materials for anodes, so it is important to consider their role in full cells for applications in electric vehicles. Here, we systematically evaluate the chemical and physical properties of six commerciallyavailable natural and synthetic graphites to establish which factors have the greatest impact on the cycling stability of full cells with nickel-rich LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes. Electrochemical data and post-mortem characterization explain the origin of capacity fade. The NMC811 cathode shows large irreversible capacity loss and impedance growth, accounting for much of full cell degradation. However, six graphite anodes demonstrate significant differences with respect to structural change, surface area, impedance growth, and SEI chemistry, which impact overall capacity retention. We found long cycle life correlated most strongly with stable graphite crystallite size. In addition, graphites with lower surface area generally had higher coulombic efficiencies during formation cycles, which led to more stable long-term cycling. The best graphite screened here enables a capacity retention around 90% in full pouch cells over extensive long-term cycling compared to only 82% for cells with the lowest performing graphite. The results show that optimal graphite selection improves cycling stability of high energy lithium-ion cells. With the booming demands for electric vehicles and electronic devices, high energy density lithium-ion batteries with long cycle life are highly desired. Despite the recent progress in Si 1 and Li metal 2 as future anode materials, graphite still remains the active material of choice for the negative electrode. 3,4 Lithium ions can be intercalated into graphite sheets at various stages like Li x C 12 and Li x C 6 , providing a high specific capacity of 372 mAh/g (∼2.5 times higher than LiCoO 2 ) and high volumetric capacity (similar to LiCoO 2 ) corresponding to LiC 6 . 5,6 In addition to its low cost and non-toxicity, graphite has a lowest average voltage (150 mV vs. Li/Li + ) and the flat voltage profile, rendering a high overall cell voltage. 7 Graphite also displays a very low voltage hysteresis, which in turn results in high energy efficiency. 8 For applications in lithium-ion batteries, many properties of the graphite powders must be optimized including crystallinity, particle size, morphology, and surface chemistry. However, most research effort has been placed on the development and characterization of high performance cathodes, while the impact of the graphite anode on full cell performance has been largely unexplored.Compared to widely used battery cathodes such as LiCoO 2 (140 mAh/g), LiFePO 4 (160 mAh/g), LiNi 1/3 Mn 1/3 Co 1/3 O 2 (160 mAh/g), and LiNi 0.5 Mn 0.3 Co 0.2 O 2 (175 mAh/g), 9-11 nickel-rich LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) is delivers a higher specific capacity (180-220 mAh/g), which increases the battery life on a single charge. 12,13 The high capacity arises because Ni is the main red...

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Section: Resultsmentioning

confidence: 92%

Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries

Mao

Wood

David

et al. 2018

J. Electrochem. Soc.

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“…100,101 This complex interplay among electrolyte degradation, phase changes, and transition metal dissolution from the cathode surface have spurred investigations of the cathode electrolyte interface (CEI) in recent years. 102 Electrolyte decomposition products deposit on the cathode surface in the form of Li 2 CO 3 , LiOH, LiF, Li x POF y , polycarbonates, and species specific to electrolyte and cathode compositions. 103,104 Strategies to improve the surface properties include doping, 105 surface coatings, 106,107 and electrolyte additives.…”

Section: High-voltage Cathode Materialsmentioning

confidence: 99%

Toward Low-Cost, High-Energy Density, and High-Power Density Lithium-Ion Batteries

Ruther

et al. 2017

JOM

224

136

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Reducing cost and increasing energy density are two barriers for widespread application of lithium-ion batteries in electric vehicles. Although the cost of electric vehicle batteries has been reduced by $70% from 2008 to 2015, the current battery pack cost ($268/kWh in 2015) is still >2 times what the USABC targets ($125/kWh). Even though many advancements in cell chemistry have been realized since the lithium-ion battery was first commercialized in 1991, few major breakthroughs have occurred in the past decade. Therefore, future cost reduction will rely on cell manufacturing and broader market acceptance. This article discusses three major aspects for cost reduction: (1) quality control to minimize scrap rate in cell manufacturing; (2) novel electrode processing and engineering to reduce processing cost and increase energy density and throughputs; and (3) material development and optimization for lithium-ion batteries with high-energy density. Insights on increasing energy and power densities of lithium-ion batteries are also addressed.

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“…59,60 F, R and T represent Faraday's constant, the universal gas constant and the absolute temperature, respectively. Specific values for i 0,SEI will be given in the Results and discussion section by Equation 11.…”

Section: Model Developmentmentioning

confidence: 99%

A SEI Modeling Approach Distinguishing between Capacity and Power Fade

Kindermann

Keil

Frank

et al. 2017

J. Electrochem. Soc.

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In this paper we introduce a pseudo two-dimensional (P2D) model for a common lithium-nickel-cobalt-manganese-oxide versus graphite (NCM/graphite) cell with solid electrolyte interphase (SEI) growth as the dominating capacity fade mechanism on the anode and active material dissolution as the main aging mechanism on the cathode. The SEI implementation considers a growth due to non-ideal insulation properties during calendar as well as cyclic aging and a re-formation after cyclic cracking of the layer during graphite expansion. Additionally, our approach distinguishes between an electronic (σ SEI ) and an ionic (κ SEI ) conductivity of the SEI. This approach introduces the possibility to adapt the model to capacity as well as power fade. Simulation data show good agreement with an experimental aging study for NCM/graphite cells at different temperatures introduced in literature. © The Author Lithium-ion batteries are one of the most promising candidates for energy storage in future stationary storage systems and electric vehicles.1-3 Enormous research efforts have been conducted to get a thorough understanding of the system "lithium-ion cell" and to further develop it for higher energy and power density, higher safety standards as well as longer cycle life. 4 The aging behavior of lithium-ion batteries has been a focus issue of battery research since the introduction of lithium-ion cells by Sony in 1991. 5 Reviews by Agubra et al., 6,7 Arora et al., 8 Aurbach et al., 9,10 Birkl et al., 11 Broussely et al., 12 Verma et al. 13 and Vetter et al. 14 are just a few examples of the extensive literature regarding aging behavior. Commonly accepted and experimentally verified aging phenomena as mentioned in the previously cited literature are electrolyte decomposition leading to solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) growth, solvent co-intercalation, gas evolution with subsequent cracking of particles, a decrease of accessible surface area and porosity due to SEI growth, contact loss of active material particles due to volume changes during cycling, binder decomposition, current collector corrosion, metallic lithium plating and transition-metal dissolution from the cathode. The listed aging mechanisms can be assigned to three different categories that are a loss of lithium-ions (LLI), an impedance increase and a loss of active material (LAM). 12,[15][16][17][18] The LLI is synonymous to a decrease in the amount of cyclable lithium-ions as they are trapped in a passivating film on either of the electrodes or in plated metallic lithium. Due to the growth of the passivating layers and/or the formation of rock-salt in the cathode (residue of the cathode active material after transition-metal dissolution), kinetic transport of lithium-ions through those inactive areas is limited and results in an impedance rise. An LAM can be caused by the dissolution of transition-metal-ions from the cathode bulk material, changes in the electrode composition and/or changes in crystal structure of the a...

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Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights

Cited by 878 publications

References 235 publications

Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries

Selecting the Best Graphite for Long-Life, High-Energy Li-Ion Batteries

Toward Low-Cost, High-Energy Density, and High-Power Density Lithium-Ion Batteries

A SEI Modeling Approach Distinguishing between Capacity and Power Fade

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