Multifunctional Ultrathin Ti3C2Tx MXene@CuCo2O4 /PE Separator for Ultra-High-Energy-Density and Large-Capacity Lithium-Sulfur Pouch Cells

Zimo Huang; Yuhao Liang; Zhenzhen Wu; Yang Kong; Maohui Bai; Meng Li; Bo Hong; Taiyu Huang; Senchuan Huang; Hao Chen; Shanqing Zhang

doi:10.1002/adma.202410318

Multifunctional Ultrathin Ti₃C₂T_x MXene@CuCo₂O₄ /PE Separator for Ultra-High-Energy-Density and Large-Capacity Lithium-Sulfur Pouch Cells

Adv Mater. 2024 Nov 12:e2410318. doi: 10.1002/adma.202410318. Online ahead of print.

Authors

Zimo Huang^{1

2}, Yuhao Liang^{1

2}, Zhenzhen Wu³, Yang Kong⁴, Maohui Bai⁵, Meng Li^{1

2}, Bo Hong⁶, Taiyu Huang⁶, Senchuan Huang^{1

2}, Hao Chen^{1

2}, Shanqing Zhang^{1

2

3}

Affiliations

¹ Institute for Sustainable Transformation, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, China.
² Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang, 515200, China.
³ Centre for Catalysis and Clean Energy, School of Environment and Science, Gold Coast Campus, Griffith University, Gold Coast, QLD, 4222, Australia.
⁴ Science Center for Material Creation and Energy Conversion, Institute of Frontier and Interdisciplinary Science, Shandong University, Qingdao, 266237, China.
⁵ College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha, 410004, China.
⁶ School of Metallurgy and Environment, Central South University, Changsha, 410083, China.

PMID: 39529518
DOI: 10.1002/adma.202410318

Abstract

The shuttling of lithium polysulfides (LiPSs), sluggish reaction kinetics, and uncontrolled lithium deposition/stripping remain the main challenges in lithium-sulfur batteries (LSBs), which are aggravated under practical working conditions, i.e., high sulfur loading and lean electrolyte in large-capacity pouch cells. This study introduces a Ti₃C₂T_x MXene@CuCo₂O₄ (MCC) composite on a polyethylene (PE) separator to construct an ultrathin MXene@CuCo₂O₄/PE (MCCP) film. The MCCP functional separator can deliver superior LiPSs adsorption/catalysis capabilities via the MCC composite and regulate the Li⁺ deposition through a conductive Ti₃C₂T_x MXene framework, enhancing redox kinetics and cycling lifetime. When paired with sulfur/carbon (S/C) cathode and lithium metal anode, the resultant 10 Ah-level pouch cell with the ultrathin MCCP separator achieves an energy density of 417 Wh kg^-1 based on the whole cell and a stable running of 100 cycles under practical operation conditions (cathode loading = 10.0 mg cm^-2, negative/positive areal capacity ratio (N/P ratio) = 2, and electrolyte/sulfur weight ratio (E/S ratio) = 2.6 µL mg^-1). Furthermore, through a systematic evaluation of the as-prepared Li-S pouch cell, the study unveils the operational and failure mechanisms of LSBs under practical conditions. The achievement of ultrahigh energy density in such a large-capacity lithium-sulfur pouch cell will accelerate the commercialization of LSBs.

Keywords: high‐energy‐density; lithium dendrites; lithium‐sulfur batteries; multifunctional separator; polysulfides shuttling.

Abstract

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