Hydrothermal Sol–Gel Synthesis of Monolithic Pyrrolic N‐Doped Carbon Gels

ABSTRACT Developing scalable strategies for carbon materials that simultaneously incorporate covalently bonded frameworks and chemically tunable surfaces remains a significant challenge. Here, we report a straightforward hydrothermal sol–gel process utilizing glucose and pyrrole precursors to produce monolithic N‐doped carbon gels (MNCGs). By controlling synthesis duration, the morphology is precisely tuned from quantum dots to macroscopic monolithic hydrogels. The primary building blocks are 5 nm hydrophilic carbon dots featuring crystalline graphitic cores and amorphous shells with 2–10 wt.% nitrogen doping, predominantly composed of pyrrolic‐N species (up to 80.21%). Following thermal activation at 700°C, MNCGs with a specific surface area of 448.72 m 2 /g and a pore volume of 0.50 cm 3 /g are obtained. Notably, the resulting gels demonstrate exceptional mechanical integrity, achieving a compressive strength of 1.42 m Pa and a wear resistance of 95.83%. These robust monolithic frameworks provide significant advantages in noble metal catalysis, effectively preventing nanoparticle sintering, and in supercapacitors, exhibiting a high specific capacitance of 221.9 F/g (at 1 A/g) with a 61% retention rate at 100 A/g. This strategy resolves the traditional trade‐off between structural integrity and surface functionality.