Ion transport behaviors are central to ion separation, micro-/nano-fluidics, and interfacial catalysis, yet achieving high ion transport rate and selectivity remains challenging in nonaqueous systems. Here, we propose a unique solid–liquid cooperative interface built from a layered cyano-bridged metal framework (CMF) and nonaqueous solvents to simultaneously increase cation (Li⁺) conductivity (9.5 mS·cm⁻¹) and transport selectivity (~0.9). Mechanistic analysis based on theoretical calculations, supported by electrochemical measurements, shows that the nonaqueous solvents can work as functional interfacial ligands at the surface of layered CMFs, including outer-layer solvent ligands (OSLs) and interlayer solvent ligands (ISLs), which can restructure the interfacial Li⁺ migration environment and salt speciation. It is found that OSLs with higher polarity symmetry would interact more strongly with the unsaturated metal sites on the CMF's surface, thereby promoting coordination competition at the interface, accelerating solvation-renewal dynamics, and increasing the Li⁺ transport rate. ISLs with higher polarity symmetry could stabilize a low-curvature surface of CMF, strengthen anion anchoring at the unsaturated metal sites, increase selectivity for Li⁺ transport, and further improve overall Li⁺ transport rate. Therefore, we provide a potential strategy to construct a unique solid-liquid interface using CMF solids and rationally designed interfacial solvent ligands to promote the ion transport behaviors.

The growing concern for the exhaustion of fossil energy and the rapid revolution of electronics have created a rising demand for electrical energy storage devices with high energy density, for example, lithium secondary batteries (LSBs). With high surface area, low cost, excellent mechanical strength, and electrochemical stability, amorphous carbon-based materials (ACMs) have been widely investigated as promising platform for anode materials in the LSBs. In this review, we firstly summarize recent advances in the synthesis of the ACMs with various morphologies, ranging from zero- to three-dimensional structures. Then, the use of ACMs in Li-ion batteries and Li metal batteries is discussed respectively with the focus on the relationship between the structural features of the as-prepared ACMs and their roles in promoting electrochemical performances. Finally, the remaining challenges and the possible prospects for the use of ACMs in the LSBs are proposed to provide some useful clews for the future developments of this attractive area.

Lithium-sulfur batteries have attracted significant attention recently due to their high theoretical capacity, energy density and cost effectiveness. However, sulfur cathodes suffer from issues such as shuttle effects, uncontrollable deposition of lithium sulfides species, and volume expansion of sulfur, which result in rapid capacity fading and low Coulombic efficiency. In recent years, metal-oxide nanostructures have been widely used in Li-S batteries, owing to their effective inhibition of the shuttle effect and controlled deposition of lithium sulfide. However, the nonconductive metal-oxides used in Li-S batteries suffer from extra diffusion process, which slows down the electrochemical reaction kinetics. Herein, we report the synthesis of carbon nanoflakes decorated with conductive aluminium-doped zinc oxide (AZO@C) nanoparticles, through a facile biotemplating method using kapok fibers as both the template and carbon source. A sulfur cathode based on the AZO@C nanocomposites shows better electrochemical performance than those of cathodes based on ZnO and Al₂O₃ with poor conductivity, with a stable capacity of 927 mAh·g^-1 at 0.1C (1C = 1, 675 mA·g^-1) after 100 cycles. A reversible capacity of 544 mAh·g^-1 after 300 cycles was obtained even after increasing the current density to 0.5C, with a 0.039% capacity decay per cycle under a sulfur loading of 3.3 mg·cm^-2. Moreover, a capacity of 466 mAh·g^-1 after 100 cycles at 0.5C could still be obtained when the sulfur loading was increased to 6.96 mg·cm^-2. The excellent electrochemical performance of the AZO@C/S composite can be attributed to its high conductivity of the polar AZO host, which suppresses the shuttle effect while simultaneously improving the redox kinetics in the reciprocal transformation of lithium sulfide species.