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Abstract

“C₂N”-species have emerged as a promising material with carbon-like applications in sorption, gas separation and energy storage, while with much higher polarity and functionality. Controlled synthesis of “C₂N” structure is still based on complex and less-sustainable monomers, which prohibits its broader industrial application. Here we report a class of well-defined C₂(N_xO_yS_z)₁ carbons with both high content of N/O/S heteroatoms and large specific surface area of up to 1704 m² g⁻¹, which can be efficiently synthesized through a simple additive condensation process using simple gallic acid and thiourea as the building blocks, without sub-tractive activation. This 1,4-para tri-doped C₂(N_xO_yS_z)₁ structure leads to sufficient CO₂ adsorption capacity (3.0 mmol g⁻¹ at 273 K, 1 bar) and a high CO₂/N₂ selectivity (47.5 for a 0.15/0.85 CO₂/N₂ mixture at 273 K). Related to the polarity, the polar frameworks can be used as supercapacitor electrodes, with record specific capacitances as high as 255 F g⁻¹at 3.5 V for a symmetric supercapacitor in ionic liquid electrolyte. This work discloses a general way for preparing a novel family of multifunctional, high heteroatom-doped porous materials for various applications.