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

• Published in: Advanced functional materials 2024-07, Vol.34 (29), p.n/a
• Main Authors: Guo, Peiting, Zhao, Ruizheng, Zhang, Zekai, Li, Jinying, Zhang, Wei, Wang, Aixia, Kang, Tianke, Lian, Cheng, Guo, Ziyang, Wang, Jin, Zhang, Jiangwei, Ma, Yuzhu
• Format: Article
• Language: English
• Subjects: Assembly; asymmetric nanoparticles; Asymmetry; Carbon; Diffusion rate; droplet; Droplets; Electrochemical analysis; Electrode materials; Flux density; hierarchical pore structure; Ion diffusion; mesoporous materials; Morphology; Nanoparticles; Nonaqueous electrolytes; Porous materials; Synthesis; Trimethylbenzene; Zinc chloride
• ISSN: 1616-301X; 1616-3028
• DOI: 10.1002/adfm.202400503

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 m2 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 ZnCl2 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. Semifootball‐like carbon nanoparticles with multimodal macro/mesopore architectures are fabricated via the droplet‐directed anisotropic assembly approach. The assembly behavior of micelles can be controlled by regulating the properties of the emulsion interface, thus transforming the particle morphology and pore structures. The tailored different pore structures provide a platform for studying the structure–activity relationships between pore composition and electrochemical properties.