Supramolecular gel-derived NiCo-N-doped porous carbon/CNT hybrid-modified separator enabling enhanced polysulfide redox kinetics and effective shuttle suppression in lithium–sulfur batteries

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RSC Adv., 2026, 16,22938-22948DOI: 10.1039/D6RA01599A, Paper Open Access &nbsp This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.Kyu Sang Lee, Taeyoung Jung, Youngseul Cho, Godeung Park, Hyunsoo Lim, Seonmin Kim, Churl Seung L…

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Supramolecular gel-derived NiCo-N-doped porous carbon/CNT hybrid-modified separator enabling enhanced polysulfide redox kinetics and effective shuttle suppression in lithium–sulfur batteries

* Corresponding authors

a Department of Applied Bioengineering, Graduate School of Convergence Science and Technology, Seoul National University, 145 Gwanggyo-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do, Republic of Korea
E-mail: [email protected]

b Advanced Battery Research Center, Korea Electronics Technology Institute (KETI), 25, Saenari-ro, Bundang-gu, Seongnam-si, Gyeonggi-do 13509, Republic of Korea

c ITC Nano Convergence Technology Research Center, Korea Electronics Technology Institute (KETI), 25, Saenari-ro, Bundang-gu, Seongnam-si, Gyeonggi-do 13509, Republic of Korea

d Program in Nano Science and Technology, Graduate School of Convergence Science and Technology, Seoul National University, 145 Gwanggyo-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do, Republic of Korea

e Department of Chemical and Biomolecular Engineering, Yonsei University, Seoul 03722, Republic of Korea

Abstract

In lithium–sulfur batteries, separator modification is a promising approach to suppress the migration of polysulfides and accelerate reaction kinetics. Herein, we propose a supramolecular gel pyrolysis-derived strategy to synthesize a NiCo-N-doped porous carbon/carbon nanotube hybrid (NiCo-NPC/CNT) for separator modification. The supramolecular gel-derived synthesis produces a three-dimensional (3D) porous carbon architecture that effectively anchors the NiCo alloy nanoparticles. Subsequently, the NiCo alloy nanoparticles act as catalysts to induce the in situ growth of carbon nanotubes during pyrolysis, thereby enhancing electrical conductivity and catalytic activity. These structural features synergistically promote physical adsorption and chemical catalytic ability, thereby accelerating the redox reactions of polysulphides. The NiCo-NPC/CNT-modified separator (NiCo-NPC/CNT@PP) cell exhibited remarkable rate capability (890.4 mAh g−1 at 3C) and cycling stability (649.0 mAh g−1 after 500 cycles at 1C). Furthermore, NiCo-NPC/CNT@PP shows excellent cycling stability under high sulfur loading (11 mg cm−2) and lean-electrolyte condition (6 µL mg−1), retaining 269.6 mAh g−1 after 120 cycles at 0.2C.