Journal
SMALL
Volume 16, Issue 47, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202004806
Keywords
heterocatalysts; layered porous carbons; lithium– sulfur batteries; metal– organic‐ frameworks; polar mediators
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Funding
- National Research Foundation of Korea (NRF) - Ministry of Science and ICT [2019R1A2B5B02070203]
- Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) - Ministry of Science and ICT [2018M3D1A1058744]
- Korea University Grant
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Although lithium-sulfur batteries exhibit a fivefold higher energy density than commercial lithium-ion batteries, their volume expansion and insulating nature, and intrinsic polysulfide shuttle have hindered their practical application. An alternative sulfur host is necessary to realize porous, conductive, and polar functions; however, there is a tradeoff among these three critical factors in material design. Here, the authors report a layered porous carbon (LPC) with VO2/V3S4 heterostructures using one-step carbonization-sulfidation of metal-organic framework templates as a sulfur host that meets all the criteria. In situ conversion of V-O ions into V3S4 nuclei in the confined 2D space generated by dynamic formation of the LPC matrix creates {200}-facet-exposed V3S4 nanosheets decorated with tiny VO2 nanoparticles. The VO2/V3S4 @ LPC composite facilitates high sulfur loading (70 wt%), superior energy density (1022 mA h g(-1) at 0.2 C, 100 cycles), and long-term cyclability (665 mA h g(-1) at 1 C, 1000 cycles). The enhanced Li-S chemistry is attributed to the synergistic heterocatalytic behavior of polar VO2 and conductive V3S4 in the soft porous LPC scaffold, which accelerates polysulfide adsorption, conversion, and charge-transfer ability simultaneously.
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