Unravelling the Secret of Sulfur Confinement and High Sulfur Utilization in Hybrid Sulfur-Carbons
Tim Horner (Max Planck Institute of Colloids and Interfaces, Potsdam)
Enis Oğuzhan Eren (Max Planck Institute of Colloids and Interfaces, Potsdam)
Elif Begüm Yılmaz (Max Planck Institute of Colloids and Interfaces, Potsdam)
Jiyong Kim (Fraunhofer Institute for Applied Polymer Research IAP, Potsdam)
Ernesto Scoppola (Max Planck Institute of Colloids and Interfaces, Potsdam)
Alexandros Vasileiadis (TU Delft - RST/Storage of Electrochemical Energy)
Nadezda V. Tarakina (Max Planck Institute of Colloids and Interfaces, Potsdam)
Markus Antonietti (Max Planck Institute of Colloids and Interfaces, Potsdam)
Evgeny Senokos (Max Planck Institute of Colloids and Interfaces, Potsdam)
undefined More Authors (External organisation)
More Info
expand_more
Other than for strictly personal use, it is not permitted to download, forward or distribute the text or part of it, without the consent of the author(s) and/or copyright holder(s), unless the work is under an open content license such as Creative Commons.
Abstract
Understanding sulfur confinement and chemical transformation in hybrid sulfur-carbon materials is critical for advancing metal-sulfur batteries. Here, we investigate the structural evolution of a sulfur-rich polymer into a hybrid sulfur-carbon via inverse vulcanization and thermal condensation. Multiscale analyses reveal a stepwise transformation, beginning with the emergence of sulfur radicals at ∼175°C, followed by the progressive development of a carbon matrix above 300°C that stabilizes the radical species. Around 450°C, a transitional phase forms, consisting of conjugated carbon clusters covalently bonded to sulfur chains. This hybrid structure confines sulfur within pseudo-graphitic nanodomains, effectively suppressing polysulfide dissolution and enhancing redox stability. DFT simulations show how sulfur confinement modulates Na-S reaction energetics, while electrochemical testing confirms high sulfur utilization, delivering ∼1000 mAh (Formula presented.) and 1200 Wh (Formula presented.), setting a new performance benchmark for room-temperature Na─S batteries. These findings provide critical insights into the correlation between structural evolution and electrochemical performance, offering design principles for next-generation sulfur-based electrodes.
help_outline