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• Single atom catalyst with Co-N 4 coordination has been precisely synthesized. • The interconnected 2D network can alleviate the formation of Li-dendrites. • Co-N 4 center suppress the shuttle effect and reduce the reaction energy barrier. • The correlation between the Co-N 4 sites and catalytic activity is deciphered. • The batteries exhibit superior electrochemical performance. Developing electrocatalyst to ameliorate the shuttling effect of lithium polysulfides (LiPSs), sluggish sulfur redox reaction kinetics and the rampant dendrite growth is of paramount importance for lithium-sulfur (Li-S) batteries. Yet still, the utilization of the most mainstream traditional metal electrocatalytic nanoparticles is far below expectation. Herein, we engineer an exclusive single-atom catalyst with planar Co-N 4 coupling of nitrogen-doped graphene mesh (SA-Co/NGM) to achieve exceptional atom utilization efficiency for catalytic conversion of LiPSs. High surface area and ultra-thin two-dimensional texture can not only accommodate high concentration monodispersed lithiophilic atomic Co sites, but also guarantee homogenize high-flux Li ion transport, alleviating the formation of Li-dendrites. Critically, the maximized exposure of Co-N 4 as a regulator in sulfur electrochemistry can conspicuously suppress the shuttle effect and accelerate bidirectional sulfur redox kinetics via electron delocalization, as demonstrated by a judicious combination of electro-kinetic analysis, in situ spectroscopy and density functional theory (DFT) computations. As expected, the batteries based on a SA-Co/NGM modified separator achieve an ultrahigh rate capability, exceptionally long cycle life and a distinguished favorable areal capacity under high sulfur loading. This work provides a rational design of single-atom catalysts for kinetics-boosted electrocatalysis towards long-lasting Li-S batteries. [ABSTRACT FROM AUTHOR]

• A three-dimensional Ni,Co-embedded CNT-coated N-doped hollow porous carbon (Ni/Co-CNT/NHPC) cathode has been designed and prepared for lithium-sulfur battery. • The Ni/Co-CNT/NHPC-S cathode possesses a high specific capacity of 1352 mA h g-1 and an excellent cycle stability at 1 C with low capacity decay of 0.094% per cycle over 500 cycles. • The mechanism of suppressing the shuttle effect on the cathode materials is discussed by analyzing adsorption experiments and density functional theory（DFT）calculation. Lithium-sulfur (Li-S) batteries have attracted great attentions due to their high specific capacity. However, the poor cycle stability caused by polysulfide shuttles, volume expansion and formation of lithium dendrites limit their practical applications. In the present work, to tackle the poor stability and unstable rate capability, a MOF-doping strategy is developed to construct a hollow porous carbon framework，which consists of Ni, Co particles and CNT on a N-doped shell surface (Ni/Co-CNT/NHPC). This hollow framework increases the load of S, slows down the volume changes, and can physically entrap soluble polysulfide. It is found that the CNT-coated network structure is beneficial for optimizing the conductivity and wettability of the material, which accelerates the reaction kinetics. Moreover, synergistic effect of abundant defects and Ni, Co nanoparticles strengthens the chemisorption of polysulfides, which suppresses the shuttle effect. As a consequence, the Ni/Co-CNT/NHPC-S cathode harvests a high specific capacity (1352 mA h g-1), and shows an excellent cycling stability at 1 C with low capacity decay of 0.094% over 500 cycles. [ABSTRACT FROM AUTHOR]