Elucidating the Performance Limitations of Lithium-ion Batteries due to Species and Charge Transport through Five Characteristic Parameters

Jiang, Fangming; Peng, Peng

doi:10.1038/srep32639

Cited by 117 publications

(92 citation statements)

References 59 publications

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“…Although, increasing the electrode thickness significantly enhances the specific capacity of the electrode up to approximately 100 µm, theoretical [19,[29][30][31][32][33][34] and experimental [35][36][37][38] results clearly show that large electrode thicknesses lead to low rate capability originating from Li + diffusion limitations in the electrolyte. For example, the conductive additive content can be increased until limitations of the electron transport in the composite become negligible.…”

mentioning

confidence: 95%

Diffusion‐Limited C‐Rate: A Fundamental Principle Quantifying the Intrinsic Limits of Li‐Ion Batteries

Heubner

Schneider

Michaelis

2019

Advanced Energy Materials

133

103

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carried out to improve the energy density at the cell level, such as the development of high capacity anode [8,9] and cathode [10,11] materials, improvements of the electrode design [12,13] and composition [14][15][16] as well as optimization of the cell architecture. [17,18] Moreover, researchers analyzed the rate limiting factors of electrodes for LIBs in great detail to understand the complex charge transport and transfer reaction processes and optimize materials and cell components accordingly. [19] It has been found that the rate performance can be improved by increasing solid-state diffusivity, [20] conductive additive type and content [21] or electrode porosity, [22] by the optimization of electrolyte properties, such as concentration [23] and viscosity, [24] and by decreasing the particle size of active materials [13,25] and the electrode thickness. [26][27][28] Although these measures lead to a gradual improvement of decisive performance metrics, a tradeoff between energy and power density became obvious, forbidding arbitrary combinations of high storage capacity and fast charging capability. Understanding this tradeoff and the accompanied practical limits of LIBs is critical for their further improvement and the development of "beyond Li" battery technologies.Herein, we present a simple but powerful electrochemical principle describing the tradeoff between storage capacity and rate capability of electrodes for LIBs. Such electrodes are porous composites consisting of particles of the active storage material, binder and conductive additives coated on a metallic current collector foil. The pores are filled with a liquid electrolyte containing Li-ions as charge carriers. The specific capacity (energy density equivalent) of such an electrode is given by the specific capacity of the active material and its share in the electrode. Figure 1 illustrates the sensitivity of the specific capacity to the most decisive electrode parameters using a typical LiNi 1/3 Mn 1/3 Co 1/3 O 2 (NCM111)-based cathode as the baseline (see Section S3 in the Supporting Information for details on the computations). Please note that here the specific capacity of the electrode also includes the masses of conductive additives, binder, current collector and the pore electrolyte, which is often ignored in the literature but has significant impact on the energy density (see Section S2 in the Supporting Information for details). It turns out that some electrode properties hardly affect the energy density, such as the porosity, the conductive additive and binder content, and the particle size (cf. Figure 1).The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/aenm.201902523.Li-ion batteries (LIBs) were continuously improved over the last decades, aiming at longer operating times of mobile electronic devices and mass implementation in high-energy applications, such as all-electric or hybrid-electric vehicles. [1][2][3][4] However, owing to safety concerns, range limitations, and inad...

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mentioning

confidence: 95%

Diffusion‐Limited C‐Rate: A Fundamental Principle Quantifying the Intrinsic Limits of Li‐Ion Batteries

Heubner

Schneider

Michaelis

2019

Advanced Energy Materials

133

103

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show abstract

“…Nevertheless, the Li-ion transport limitations in liquid electrolytes become increasingly important as the electrode thickness increases 67,68,70,71 because the diffusion time in the liquid phase is no longer negligible as a result of the significant increase in diffusion length in the thick porous electrodes. Consequently, it is necessary to design thick electrode architectures to take advantage of the increased energy density provided by the higher active material volume ratio, while minimizing the tortuosity and transport limitations that can be detrimental to power performance.…”

Section: Electrode Engineeringmentioning

confidence: 99%

“…Many different designs have been suggested, including graded-porosity and hierarchical architectures, 67,[72][73][74][75][76] and several simulations have shown that smaller active material particles can help decrease the polarization and capacity loss observed at high discharge rates by shortening the Li-ion diffusion path in the particles. 68,71,77 Yet, particle size variations also affect the packing structure of the electrode and can result in different pore sizes and distributions, as well as in differences in the contact resistance between the electrode and the current collector. These variations could be leveraged to improve transport properties and battery performance.…”

Section: Electrode Engineeringmentioning

confidence: 99%

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

Ruther

et al. 2017

JOM

232

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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“…The first rapid decline is in response to the fast decreasing SOC; for the 4 mΩ case, the discharge current is too large, making this period too short to observe. In the middle period, the discharge process is limited by the lithium transport in the electrolyte or in solid active materials . Regarding the last instant drop period, we speculate it is caused by the destroyed or blocked Li‐ion transmission pathways in the battery inside rather than the disconnection of electricity circuit.…”

Section: Resultsmentioning

confidence: 94%

“…In the middle period, the discharge process is limited by the lithium transport in the electrolyte or in solid active materials. 14,20,21 Regarding the last instant drop period, we speculate it is caused by the destroyed or blocked Li-ion transmission pathways in the battery inside rather than the disconnection of electricity circuit. The high temperature (Figure 3 C) may arouse some abusive reactions of the battery materials (several reactions are involved for an overheated cell) inside the battery, which consume some battery materials or destroy the internal structure.…”

Section: Effects Of Esc Resistancementioning

confidence: 97%

Electrical‐thermal behaviors of a cylindrical graphite‐NCA Li‐ion battery responding to external short circuit operation

et al. 2019

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Summary Large amount of heat generated during an external short circuit (ESC) process may cause battery safety events. An experimental platform is established to explore the battery electrothermal characteristics during ESC faults. For 18650‐type nickel cobalt aluminum (NCA) batteries, ESC fault tests of different initial state of charge (SOC) values, different external resistances, or different ambient temperatures are carried out. The test case of a smaller external resistance is characterized by a shorter ESC duration with a faster cell temperature rise, whereas the case of a larger external resistance will last for a longer duration, discharge more electricity, and terminate in a slightly higher temperature. The tested batteries of high initial SOCs generally have higher temperature rise rates, smoother changes at the output current/voltage curves, but a smaller discharged capacity. The batteries of low initial SOCs can be overdischarged by the ESC operations. At low temperatures, say 0°C, the ESC process outputs much less electricity than the process at high temperatures, eg, 30°C. The initial low temperature has little effect on reducing the battery overheat due to ESC operations. The battery thermal behavior is of hysteresis property; analysis of heat generations reveals the subsequent increase of battery surface temperature after the completion of ESC discharge is due to the battery material abusive reaction heats. It is found from analytical and numerical analyses that there can have approximately 30°C temperature difference between the battery core and its surface during ESC operations. The interruption of ESC operation is very probably caused by the high battery core temperature, which leads to the destruction of solid‐electrolyte interface (SEI) film.

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Elucidating the Performance Limitations of Lithium-ion Batteries due to Species and Charge Transport through Five Characteristic Parameters

Cited by 117 publications

References 59 publications

Diffusion‐Limited C‐Rate: A Fundamental Principle Quantifying the Intrinsic Limits of Li‐Ion Batteries

Diffusion‐Limited C‐Rate: A Fundamental Principle Quantifying the Intrinsic Limits of Li‐Ion Batteries

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

Electrical‐thermal behaviors of a cylindrical graphite‐NCA Li‐ion battery responding to external short circuit operation

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