2,5‐Dimercapto‐1,3,4‐Thiadiazole (DMCT)‐Based Polymers for Rechargeable Metal–Sulfur Batteries

Bhargav, Amruth; Manthiram, Arumugam

doi:10.1002/eem2.12446

2,5‐Dimercapto‐1,3,4‐Thiadiazole (DMCT)‐Based Polymers for Rechargeable Metal–Sulfur Batteries (in EN)

Journal Article · Sat Jun 03 00:00:00 EDT 2023 · Energy & Environmental Materials

DOI:https://doi.org/10.1002/eem2.12446· OSTI ID:2575888

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Univ. of Texas, Austin, TX (United States)

Organosulfur materials are a sustainable alternative to the present-day layered oxide cathodes in lithium-based batteries. One such organosulfur material that was intensely explored from the 1990s to early 2010s is 2,5-dimercapto-1,3,4-thiadiazole (DMCT). However, research interest declined as the electrode reactions with DMCT were assumed to be too sluggish to be practical. Armed with the advances in metal–sulfur batteries, we revisit DMCT-based materials in the form of poly[tetrathio-2,5-(1,3,4-thiadiazole)], referred to as pDMCT-S. With an appropriate choice of electrode design and electrolyte, pDMCT-S cathode paired with a Li-metal anode shows a capacity of 715 mA h g⁻¹ and a Coulombic efficiency of 97.7% at a C/10 rate, thus quelling the concerns of sluggish reactions. Surprisingly, pDMCT-S shows significantly improved long-term cyclability compared to a sulfur cathode. Investigations into the origin of the stability reveals that the discharge product Li-DMCT in its mesomeric form can strongly bind to polysulfides, preventing their dissolution into the electrolyte and shuttling. This unique mechanism solves a critical problem faced by sulfur cathodes. Encouragingly, this mechanism results in a stable performance of pDMCT-S with Na-metal cells as well. In conclusion, this study opens the potential for exploring other organic materials that have inherent polysulfide sequestering capabilities, enabling long-life metal–sulfur batteries.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States)

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

Grant/Contract Number:: SC0005397

OSTI ID:: 2575888

Alternate ID(s):: OSTI ID: 1957842

Journal Information:: Energy & Environmental Materials, Journal Name: Energy & Environmental Materials Journal Issue: 6 Vol. 6; ISSN 2575-0356

Publisher:: Wiley - Zhengzhou UniversityCopyright Statement

Country of Publication:: United States

Language:: EN

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