Microstructure and defect engineering of graphite anodes by pulsed laser annealing for enhanced performance of lithium-ion batteries

Khosla, Nayna; Narayan, Jagdish; Narayan, Roger; Sun, Xiao-Guang; Paranthaman, Mariappan Parans

doi:10.1016/j.carbon.2023.01.009

Title: Microstructure and defect engineering of graphite anodes by pulsed laser annealing for enhanced performance of lithium-ion batteries

Journal Article · Thu Jan 19 00:00:00 EST 2023 · Carbon

DOI:https://doi.org/10.1016/j.carbon.2023.01.009· OSTI ID:1923953

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North Carolina State University, Raleigh, NC (United States)
North Carolina State University, Raleigh, NC (United States); University of North Carolina, Chapel Hill, NC (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

We report nanosecond pulsed laser annealing significantly improves cyclability and current carrying capacity of lithium-ion batteries (LIBs). This improvement is achieved by engineering of microstructure and defect contents present in graphite in a controlled way by using pulsed laser annealing (PLA) to increase the number density of Li⁺ ion trapping sites. The PLA treatment causes the following changes: (1) creates surface steps and grooves between the grains to improve Li⁺ ion charging and intercalation rates; (2) removes inactive polyvinylidene difluoride (PVDF) binder from the top of graphite grains and between the grains which otherwise tends to block the Li⁺ migration; and (3) produces carbon vacancies in (0001) planes which can provide Li⁺ charging sites. From X-ray diffraction data, we find upshift in diffraction peak or reduction in planar spacing, from which vacancy concentration was estimated to be about 1.0%, which is higher than the thermodynamic equilibrium concentration of vacancies. The laser treatment creates single and multiple C vacancies which provide sites for Li⁺ ions, and it also produces steps and grooves for Li⁺ ions to enter the intercalating sites. It is envisaged that the formation of these sites enhances Li+ ion absorption during charge and discharge cycles. The current capacity increases from an average 360 mAh/g to 430 mAh/g, and C–V shows significant reduction in SEI layer formation after the laser treatment. If the vacancy concentration is too high and charge-discharge cycles are long, then trapping of electrons by Li⁺ may occur, which can lead to Li⁰ formation and Li plating causing reduction in current capacity.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; DMR-2016256; ECCS-2025064

OSTI ID:: 1923953

Alternate ID(s):: OSTI ID: 1922971; OSTI ID: 1997803

Journal Information:: Carbon, Vol. 205, Issue 3; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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