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Nano Research Energy https://doi.org/10.26599/NRE.2024.9120116
Research Article | Open Access | Online first | Published: 04 March 2024

Titanium-containing high entropy oxide (Ti-HEO): A redox expediting electrocatalyst towards lithium polysulfides for high performance Li-S batteries

Show Author's Information Hassan Raza1,2,§,  Junye Cheng1,§( ),  Jingwei Wang1,  Subash Kandasamy3,  Guangping Zheng2( ),  Guohua Chen3( )
Department of Materials Science, Shenzhen MSU-BIT University, Shenzhen 517182, China
Department of Mechanical Engineering, Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China
School of Energy and Environment, City University of Hong Kong, Dat Chee Avenue, Kowloon, Hong Kong SAR, China

§ Hassan Raza and Junye Cheng contributed equally to this work.

Keywords:
electrical conductivity, lithium-sulfur batteries, catalytic conversion, titanium containing high entropy oxide (Ti-HEOs), multi-metal-MOFs template method
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Raza H, Cheng J, Wang J, et al. Titanium-containing high entropy oxide (Ti-HEO): A redox expediting electrocatalyst towards lithium polysulfides for high performance Li-S batteries. Nano Research Energy, 2024, https://doi.org/10.26599/NRE.2024.9120116
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Abstract Full text Electronic supplementary material About this article

Since lithium sulfur (Li-S) energy storage devices are anticipated to power portable gadgets and electric vehicles owing to their high energy density (2600 Wh·kg–1); nevertheless, their usefulness is constrained by sluggish sulfur reaction kinetics and soluble lithium polysulfide (LPS) shuttling effects. High electrically conductive bifunctional electrocatalysts are urgently needed for Li-S batteries, and high-entropy oxide (HEO) is one of the most promising electrocatalysts. In this work, we synthesize titanium-containing high entropy oxide (Ti-HEO) (TiFeNiCoMg)O with enhanced electrical conductivity through calcining metal-organic frameworks (MOF) templates at modest temperatures. The resulting single-phase Ti-HEO with high conductivity could facilitate chemical immobilization and rapid bidirectional conversion of LPS. As a result, the Ti-HEO/S/KB cathode (with 70 wt.% of sulfur) achieves an initial discharge capacity as high as ~1375 mAh·g–1 at 0.1 C, and a low-capacity fade rate of 0.056% per cycle over 1000 cycles at 0.5 C. With increased sulfur loading (~5.0 mg·cm–2), the typical Li-S cell delivered a high initial discharge capacity of ~607 mAh·g–1 at 0.2 C and showcased good cycling stability. This work provides better insight into the synthesis of catalytic Ti-containing HEOs with enhanced electrical conductivity, which are effective in simultaneously enhancing the LPS-conversion kinetics and reducing the LPS shuttling effect.


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About this article

Titanium-containing high entropy oxide (Ti-HEO): A redox expediting electrocatalyst towards lithium polysulfides for high performance Li-S batteries

Show Author's information Hassan Raza1,2,§, Junye Cheng1,§( ), Jingwei Wang1, Subash Kandasamy3, Guangping Zheng2( ), Guohua Chen3( )
Department of Materials Science, Shenzhen MSU-BIT University, Shenzhen 517182, China
Department of Mechanical Engineering, Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China
School of Energy and Environment, City University of Hong Kong, Dat Chee Avenue, Kowloon, Hong Kong SAR, China

§ Hassan Raza and Junye Cheng contributed equally to this work.

Abstract

Since lithium sulfur (Li-S) energy storage devices are anticipated to power portable gadgets and electric vehicles owing to their high energy density (2600 Wh·kg–1); nevertheless, their usefulness is constrained by sluggish sulfur reaction kinetics and soluble lithium polysulfide (LPS) shuttling effects. High electrically conductive bifunctional electrocatalysts are urgently needed for Li-S batteries, and high-entropy oxide (HEO) is one of the most promising electrocatalysts. In this work, we synthesize titanium-containing high entropy oxide (Ti-HEO) (TiFeNiCoMg)O with enhanced electrical conductivity through calcining metal-organic frameworks (MOF) templates at modest temperatures. The resulting single-phase Ti-HEO with high conductivity could facilitate chemical immobilization and rapid bidirectional conversion of LPS. As a result, the Ti-HEO/S/KB cathode (with 70 wt.% of sulfur) achieves an initial discharge capacity as high as ~1375 mAh·g–1 at 0.1 C, and a low-capacity fade rate of 0.056% per cycle over 1000 cycles at 0.5 C. With increased sulfur loading (~5.0 mg·cm–2), the typical Li-S cell delivered a high initial discharge capacity of ~607 mAh·g–1 at 0.2 C and showcased good cycling stability. This work provides better insight into the synthesis of catalytic Ti-containing HEOs with enhanced electrical conductivity, which are effective in simultaneously enhancing the LPS-conversion kinetics and reducing the LPS shuttling effect.

Keywords: electrical conductivity, lithium-sulfur batteries, catalytic conversion, titanium containing high entropy oxide (Ti-HEOs), multi-metal-MOFs template method

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Received: 01 November 2023
Revised: 25 January 2024
Accepted: 01 February 2024
Published: 04 March 2024

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© The Author(s) 2024. Published by Tsinghua University Press.

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Acknowledgements

The authors are grateful for the following financial supports: the National Natural Science Foundation of China (Nos. 52372289 and 52102368), Guangdong Science and Technology Bureau (Grant Nos. 2019B090908001 and 2020A0505090011), Guangdong Special Fund for Key Areas (20237DZX3042), Shenzhen STI (Grant No. SGDX20190816230615451), Shenzhen Stable Support Project, Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices (Grant No. 2019B121205001), Otto Poon Charitable Foundation (Grant Nos. 847W, CDBC, CDBW), and HKPolyU Postdoctoral Fellowships (Grant No. W28H).

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