Droplet‐Directed Anisotropic Assembly of Semifootball‐Like Carbon Nanoparticles with Multimodal Pore Architectures

Abstract Hierarchical porous carbon nanoparticles, with tailored asymmetric morphologies and pore structures, have great implications in high‐performance electrode materials. However, the controlled synthesis of anisotropic carbon nanoparticles with tailored multimodal pore structures remains a challenge. Herein, a droplet‐directed anisotropic assembly approach to synthesize asymmetric carbon nanoparticles with macro/mesopores is demonstrated. This synthesis relies on the anisotropic growth of mesoporous polydopamine (PDA) seeds on the emulsion interfaces and the subsequent immersion of 1,3,5‐trimethylbenzene (TMB) droplets into the seeds. The obtained carbon nanoparticles present a semifootball‐shaped morphology with a high surface area (383 m 2 g −1 ), well‐controlled macropores (≈105 nm), and mesopores (≈3.8 nm). By tuning the polarity of the oil phase, the morphologies transform from non‐porous spheres to semifootball‐like architectures and finally to nano‐ellipsoid with meso‐channels. The pore structures are further optimized by ZnCl 2 activation, and the semifootball‐like carbon nanoparticles with modulated pore compositions deliver a high reversible capability, excellent rate performance (215 F g −1 at 0.05 A g −1 and 143 F g −1 at 20 A g −1 in organic electrolyte), and enhanced energy density (53.4 Wh Kg −1 ). Simulation results elucidate the structure–activity relationship between the multistage pore structure and electrochemical performance, i.e., pore hierarchy enhances ion diffusion flux, and large‐mesopore structure facilitates rate performance.