Covalent organic frameworks (COFs) were the promising solar catalysts for producing hydrogen peroxide (H2O2). However, they remain suffered from poor light absorption, slow charge separation, and limited substrate accessibility. To address these issues, we synthesized an imine-linked triazine-based COF directly onto carbon nanotubes (CNTs) through an interface-mediated Schiff base reaction, creating a tubular nano-complex designated as CNT@COF. Protonation of the imine bonds in the resulting CNT@COF-H significantly enhanced its photocatalytic H2O2 production, achieving a rate of 790.5 μM·h−1 under one sunlight irradiation. This performance outshines that of the unmodified COF and surpasses many other COF-based materials. Further studies revealed that protonation improved substrate accessibility, while the integrated CNTs acted as electron transporters to expand light absorption and reduce charge recombination, thereby enhancing photocatalytic activity. The efficacy of CNT@COF-H was demonstrated through its strong sterilization capability and clear dye degradation, offering a promising method for efficient and eco-friendly production of H2O2.
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Single atom catalyst is of great importance for the oxygen reduction reaction (ORR). However, facile preparation of single atom catalyst without using well-designed precursors or labor-intensive acid leaching remains an urgent challenge. Herein, a simple pyrolysis of Fe3+-loaded mesoporous phenolic resin (mPF)-melamine precursor is used to prepare the single atom iron-anchored N-doped mesoporous graphitic carbon nanospheres (Fe/N-MGN). Investigation of the synthesis reveals the appropriate Fe-assisted catalysis effect and mPF template effect, which not only spurs the highly graphitic porous framework of Fe/N-MGN with plentiful pyridinic N/graphitic N, but also assures the dispersed single atom Fe anchoring without elaborated procedures. As a result, the as-synthesized Fe/N-MGN demonstrates high catalytic activity, good durability and excellent methanol tolerance for ORR. This work promises a facile method to regulate the graphitic carbon growth and single atom Fe loading for the highly efficient electrocatalysis.
Labor-saving preparation of highly active electrocatalysts for alcohols oxidation, especially for the ethylene glycol and glycerol electrooxidation is of great importance for the development of fuel cells. Herein, mesocellular graphene foam (MGF) constructed by ultrathin nanosheets were prepared using lamellar MCM-22 zeolite as template and then ultra-small Pd NPs were facile grew on it via the stabilizer-free synthesis. Detailed characterizations showed that the obtained Pd/MGF had large surface area, hierarchical porous architecture, semi-graphitic framework and dispersed Pd NPs anchoring. Electrochemical measurements demonstrated that Pd/MGF possessed the higher catalytic activity (1.7–2.9 fold higher) and stability for the different alcohols electrooxidation, especially for the ethylene glycol and glycerol electrooxidation in the alkaline solution, than the commercial Pd/C (10 wt.%) catalyst. Reaction kinetics analysis revealed the expanded diffusion-controlled process of Pd/MGF as compared to Pd/C. These findings promised a potential electrocatalyst for direct alcohol fuel cells (DAFC), especially for the direct ethylene glycol or glycerol fuel cells with high energy density.