Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage

Wu, Jingyi; Ju, Zhengyu; Zhang, Xiao; Xu, Xiao; Takeuchi, Kenneth J.; Marschilok, Amy C.; Takeuchi, Esther S.; Yu, Guihua

doi:10.1021/acsnano.2c00129

Low-Tortuosity Thick Electrodes with Active Materials Gradient Design for Enhanced Energy Storage

Journal Article · Wed Mar 02 00:00:00 EST 2022 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.2c00129· OSTI ID:1865650

Wu, Jingyi ^[1]; Ju, Zhengyu ^[2]; ^[2]; Xu, Xiao ^[2]; ^[3]; Marschilok, Amy C. ^[3]; Takeuchi, Esther S. ^[3]; Yu, Guihua ^[2]

Univ. of Texas, Austin, TX (United States); Northwestern University, Evanston, IL, United States
Univ. of Texas, Austin, TX (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

The ever-growing energy demand of modern society calls for the development of high-loading and high-energy-density batteries, and substantial research efforts are required to optimize electrode microstructures for improved energy storage. Low-tortuosity architecture proves effective in promoting charge transport kinetics in thick electrodes; however, heterogeneous electrochemical mass transport along the depth direction is inevitable, especially at high C-rates. In this work, we create an active material gradient in low-tortuosity electrodes along ion-transport direction to compensate for uneven reaction kinetics and the nonuniform lithiation/delithiation process in thick electrodes. The gradual decrease of active material concentration from the separator to the current collector reduces the integrated ion diffusion distance and accelerates the electrochemical reaction kinetics, leading to improved rate capabilities. Further, the structure advantages combining low-tortuosity pores and active material gradient offer high mass loading (60 mg cm^–2) and enhanced performance. Comprehensive understanding of the effect of active material gradient architecture on electrode kinetics has been elucidated by electrochemical characterization and simulations, which can be useful for development of batteries with high-energy/power densities.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties; Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012673; SC0012704; SC0021314

OSTI ID:: 1865650

Alternate ID(s):: OSTI ID: 1895071

Report Number(s):: BNL--223640-2022-JAAM

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 3 Vol. 16; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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