High-energy-density Li-S batteries are considered one of the next-generation energy storage systems, but the uncontrolled Li-dendrite growth in Li metal anodes and the shuttling of polysulfides in S cathode severely impede the commercial development of Li-S batteries. Herein, a conductive composite architecture that is made up of bio-derived N-doped porous carbon fiber bundles (N-PCFs) with co-imbedded cobalt and niobium carbide nanoparticles is employed as a multifunctional integrated host for simultaneously addressing the challenges in both Li anodes and S cathodes. The implantation of Co and NbC nanoparticles bestows the N-PCFs matrix with synergistically enhanced degree of graphitization, electrical conductivity, hierarchical porosity, and surface polarization. Theoretical calculations and experimental results show that NbC with specific lithiophilic and sulfiphilic features can synchronously regulate the Li and S electrochemistry by realizing homogeneous lithium deposition with suppressed Li-dendrite growth and exerting catalytic effects for promoting the polysulfide conversion together with fast Li 2 S nucleation. Hence, the assembled Li-S full batteries exhibit a superb rate capability (704 mAh g −1 at 5 C) and cycling life (≈82.3% capacity retention after 500 cycles) at a sulfur loading over 3.0 mg cm −2 , as well as high reversible areal capacity (>6.0 mAh cm −2) even at a higher sulfur loading of 6.7 mg cm −2 .

Given the inherent features of open tunnel‐like pyrochlore crystal frameworks and pentavalent antimony species, polyantimonic acid (PAA) is an appealing conversion/alloying‐type anode material with fast solid‐phase ionic diffusion and multielectron reactions for lithium‐ion batteries. Yet, enhancing the electronic conductivity and structural stability are two key issues in exploiting high‐rate and long‐life PAA‐based electrodes. Herein, these challenges are addressed by engineering a novel multidimensional integrated architecture, which consists of 0D Mn‐substituted PAA nanocrystals embedded in 1D tubular graphene scrolls that are co‐assembled with 2D N‐doped graphene sheets. The integrated advantages of each subunit synergistically establish a robust and conductive 3D electrode framework with omnidirectional electron/ion transport network. Computational simulations combined with experiments reveal that the partial‐substitution of H3O+ by Mn2+ into the tunnel sites of PAA can regulate its electronic structure to narrow the bandgap with increased intrinsic electronic conductivity and reduce the Li+ diffusion barrier. All above merits enable improved reaction kinetics, adaptive volume expansion, and relieved dissolution of active Mn2+/Sb5+ species in the electrode materials, thus exhibiting ultrahigh rate capacity (238 mAh g−1 at 30.0 A g−1), superfast‐charging capability (fully charged with 56% initial capacity for ≈17 s at 80.0 A g−1) and durable cycling performance (over 1000 cycles).

A novel 1D hierarchical chainlike LiCoO2 organized by flake-shaped primary particles is synthesized via a facile template-engaged strategy by using CoC2O4·2H2O as a self-sacrificial template obtained from a simple coprecipitation method. The resultant LiCoO2 has a well-built hierarchical structure, consisting of secondary micrometer-sized chains and sub-micrometer-sized primary flakes, while these primary LiCoO2 flakes have specifically exposed fast-Li(+)-diffused active {010} facets. Owing to this unique hierarchical structure, the chainlike LiCoO2 serves as a stable cathode material for lithium-ion batteries (LIBs) operated at a high cutoff voltage up to 4.5 V, enabling highly reversible capacity, remarkable rate performance, and long-term cycle life. Specifically, the chainlike LiCoO2 can deliver a reversible discharge capacity as high as 168, 156, 150, and 120 mAh g(-1) under the current density of 0.1, 0.5, 1, and 5 C, respectively, while about 85% retention of the initial capacity can be retained after 200 cycles under 1 C at room temperature. Moreover, the chainlike LiCoO2 also shows an excellent cycling stability at a wide operating temperature range, showing the capacity retention of ∼73% after 200 cycles at 55 °C and of ∼68% after 50 cycles at -10 °C, respectively. The work described here suggests the great potential of the hierarchical chainlike LiCoO2 as high-voltage cathode materials aimed toward developing advanced LIBs with high energy density and power density.

HIGHLIGHTS • Flexible hierarchical electrode architecture was constructed by rooting MOF-derived CoS 2 /carbon nanoleaf arrays into a nitrogen-rich 3D conductive scaffold. • An accelerated electrocatalytic effect and improved polysulfide redox kinetics arising from the structure advantages were investigated. • As-prepared composite delivers a significantly improved electrochemical performance not only at room temperature but also at elevated temperature.

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