From Fundamental Understanding to Engineering Design of High‐Performance Thick Electrodes for Scalable Energy‐Storage Systems

Wu, Jingyi; Zhang, Xiao; Ju, Zhengyu; Wang, Lei; Hui, Zeyu; Mayilvahanan, Karthik S.; Takeuchi, Kenneth J.; Marschilok, Amy C.; West, Alan C.; Takeuchi, Esther S.; Yu, Guihua

doi:10.1002/adma.202101275

Cited by 107 publications

(87 citation statements)

References 117 publications

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“…Overall, in order to achieve high gravimetric and volumetric energy densities, assuming no material evolution, a possible way is to increase electrode thickness and therefore raise the active material ratio at the package level. However, higher overpotential in thicker electrodes has an adverse impact on the power density of thick electrodes [58]. Thus, low tortuosity seems to become the key feature of state-of-the-art electrodes with both high energy and power densities.…”

Section: Concentration Polarization In Thick Electrodesmentioning

confidence: 99%

Vertically aligned two-dimensional materials-based thick electrodes for scalable energy storage systems

Zhang

et al. 2021

Nano Res.

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Together with the blooming of portable smart devices and electric vehicles in the last decade, electrochemical energy storage (EES) devices capable of high-energy and high-power storage are urgently needed. Two-dimensional (2D) materials, benefiting from the short solid-state diffusion distance, are well recognized to possess excellent electrochemical performance. However, liquid diffusion, the rate-determining process in thick electrodes, is notably slow in 2D materials-based electrodes stemming from their stacking during electrode processing, which considerably limits their applications for high energy storage. To fully exploit intrinsic advantages of 2D materials for scalable energy storage devices, this review summarizes several important strategies, ranging from assembly to template methods, to fabricate vertically aligned 2D materials-based electrodes. We further discuss the advantages and challenges of these methods in terms of key features of thick electrodes and illustrate the design principles for high-energy/power devices.

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Section: Concentration Polarization In Thick Electrodesmentioning

confidence: 99%

Vertically aligned two-dimensional materials-based thick electrodes for scalable energy storage systems

Zhang

et al. 2021

Nano Res.

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“…Many previous studies implemented to achieve this goal were devoted to the synthesis and modification of electrode active materials and electrolytes 4 – 6 . Along with these material-based works, the design of high-mass-loading electrodes has recently garnered considerable attention as a facile and scalable architectural strategy 7 , 8 .…”

Section: Introductionmentioning

confidence: 99%

Redox-homogeneous, gel electrolyte-embedded high-mass-loading cathodes for high-energy lithium metal batteries

Kim

Cho

et al. 2022

Nat Commun

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Lithium metal batteries have higher theoretical energy than their Li-ion counterparts, where graphite is used at the anode. However, one of the main stumbling blocks in developing practical Li metal batteries is the lack of cathodes with high-mass-loading capable of delivering highly reversible redox reactions. To overcome this issue, here we report an electrode structure that incorporates a UV-cured non-aqueous gel electrolyte and a cathode where the LiNi0.8Co0.1Mn0.1O2 active material is contained in an electron-conductive matrix produced via simultaneous electrospinning and electrospraying. This peculiar structure prevents the solvent-drying-triggered non-uniform distribution of electrode components and shortens the time for cell aging while improving the overall redox homogeneity. Moreover, the electron-conductive matrix eliminates the use of the metal current collector. When a cathode with a mass loading of 60 mg cm−2 is coupled with a 100 µm thick Li metal electrode using additional non-aqueous fluorinated electrolyte solution in lab-scale pouch cell configuration, a specific energy and energy density of 321 Wh kg−1 and 772 Wh L−1 (based on the total mass of the cell), respectively, can be delivered in the initial cycle at 0.1 C (i.e., 1.2 mA cm−2) and 25 °C.

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“…Lithium-sulfur (LiS) batteries with a high theoretical capacity of 1675 mAh g −1 have been attracting attention as a next-generation energy storage device. [1][2][3] The practical application of LiS batteries is being delayed by incomplete utilization of theoretical capacity due to intrinsic obstacles related to the sulfur conversion reaction. [4][5][6][7] Specifically, during the charging/ discharging process, a solid-state product of sulfur or lithium sulfide (Li 2 S) is produced through a liquid-phase lithium polysulfide (LiPS) intermediate; the high solubility of LiPSs in the electrolyte adds diffusion limitation to the conversion reaction and the electrical/ionic non-conducting properties of sulfur and Li 2 S cause a high energy barrier to the conversion.…”

Section: Introductionmentioning

confidence: 99%

Balancing Electrolyte Donicity and Cathode Adsorption Capacity for High‐Performance LiS Batteries

Kim

Moon

2022

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LiS batteries with high theoretical capacity are attracting attention as next‐generation energy storage systems. Much effort has been devoted to the introduction of cathode materials with strong adsorption to sulfide species, but it is presented that this selection should be refined in the application of high donicity electrolytes. The oxides with different adsorption capacities are explored while controlling the electrolyte donicity, confirming the trade‐off effect between the donicity and the adsorption capacity for sulfur conversion. Specifically, a cathode substrate containing oxide nanoparticles of MgO, NiO, Fe2O3, Co3O4, and V2O5 is prepared with spectra in adsorption capacity as well as low and high donicity electrolytes by controlling the concentration of LiNO3 salt. Strong adsorbent oxides such as Co3O4 and V2O5 cause competitive adsorption of electrolyte salts in high donicity electrolytes, resulting in poor cell performance. High cell performance is achieved on weakly adsorbing oxides of MgO or NiO with high donicity electrolytes; the MgO‐containing cathode cell delivers a high discharge capacity of 1394 mAh g−1 at 0.2 C. It is believed that understanding the interactions between electrolytes and adsorbent substrates will be the cornerstone of high‐performance LiS batteries.

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From Fundamental Understanding to Engineering Design of High‐Performance Thick Electrodes for Scalable Energy‐Storage Systems

Cited by 107 publications

References 117 publications

Vertically aligned two-dimensional materials-based thick electrodes for scalable energy storage systems

Vertically aligned two-dimensional materials-based thick electrodes for scalable energy storage systems

Redox-homogeneous, gel electrolyte-embedded high-mass-loading cathodes for high-energy lithium metal batteries

Balancing Electrolyte Donicity and Cathode Adsorption Capacity for High‐Performance LiS Batteries

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