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Ambient laser-induced dual engineering of intrinsic defects and Fe-N4 sites in graphene: An electronic synergy for highly efficient lithium-sulfur batteries
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DOI：10.1016/j.jechem.2026.07.075.png)
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Abstract
En 中文
Carbon-based metal single-atom catalysts (C-SACs) are highly appealing due to their maximized atomic utilization efficiency and unique electronic properties. However, conventional high-temperature synthesis usually causes metal agglomeration, adversely affecting catalytic performance. Herein, we propose a laser-induced dual engineering strategy to achieve the stable dispersion of Fe single atoms within a defect-rich graphene framework (denoted as Fe-N-DG-2). The laser-induced high-temperature thermal shock first creates abundant intrinsic defects in graphene and subsequently triggers the implantation of Fe atoms into the graphene lattice in the Fe-N4 coordination form. The ultra-fast quenching process locks these thermodynamically non-equilibrium structures. As a proof-of-concept in lithium-sulfur (Li-S) batteries, the as-made Fe-N-DG-2 exhibits enhanced polysulfide adsorption and catalytic conversion, which are attributed to the synergistic electronic modulation between Fe-N4 moieties and the surrounding intrinsic carbon defects. Therefore, the Li-S batteries assembled with Fe-N-DG-2-modified separators deliver a high rate capacity of 830 mAh g−1 at 2 C and outstanding cycling stability over 500 cycles, with a low capacity fading rate of 0.07% per cycle at 1 C. This work not only offers a novel synthesis platform for stable C-SACs but also highlights the importance of engineering intrinsic defect structures in carbon supports for developing high-efficiency C-SACs.
Keywords:
Single-atom catalysts
Laser-induced graphene
Intrinsic carbon defects
Lithium-sulfur batteries
Shuttle effect
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