Three‐Dimensional Carbon Cloth/RGO Supported Nano‐Porous Polyoxometalate as a Catalytic Host for High‐Loading Lithium–Sulfur Batteries

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Lithium–sulfur batteries (LSBs) have emerged as one of the most prospective next‐generation rechargeable energy storage devices because of their exceptional energy densities. However, the dissolution and shuttle behavior of lithium polysulfides (LiPSs) intermediates, coupled with slow redox dynamics, have impeded their practical application. In this respect, polyoxometalates (POMs) represent a class of metal‐oxide nanoclusters capable of reversible multielectron redox and efficient LiPSs capture, which enable them to maintain the reversibility of LiPSs conversion while accelerating the redox kinetics of LiPSs. However, the poor conductivity of POMs restricts their electrochemical performance in LSBs with high sulfur loading. To address this issue, the nano‐porous K 3 PW 12 O 40 ( KPW ) is in situ grown on three‐dimensional (3D) carbon cloth@reduced graphene oxide ( CC@RGO ) conductive substrate to gain a POM‐based host material ( CC@RGO/KPW‐A ) as catalyst via the two‐step calcination strategy. This integrated architecture synergistically accelerates the redox kinetics of LiPSs and promotes rapid charge transfer in LSBs, thus significantly improving the performance. The obtained POM‐based sulfur cathode shows an initial discharge capacity of 9.6 mAh cm −2 even under a high sulfur loading of 10.2 mg cm −2 . This work provides a facile approach to boost the electrochemical properties of LSBs with high sulfur loading.