没食子酸和硫脲合成具有N,O和S排列孔的碳骨架用于高效CO2吸附和超级电容器

"C2N"是一种很有前途的材料,在吸附、气体分离和能量存储方面具有类似碳的应用,且具有更高的极性和功能性.然而,"C2N"的可控合成仍基于复杂且不可持续的单体,阻碍了其更广泛的工业应用.本文报道了一种具有特定结构的C2(NxOySz)1碳材料,即以简单的没食子酸和硫脲为结构单元,通过简单的加成缩合制备,无需活化.所制备的碳材料具有高的N/O/S杂原子含量和大的比表面积(高达1704 m^2g^-1).此1,4-对位三掺杂孔结构使得C2(NxOySz)1具有较好的CO2吸附能力(在273 K,1 bar下为3.0 mmol g^-1)和较高的CO2/N2选择性(在273 K,CO2/N2=0.15/0.85下为47.5).此外,由于碳骨架高极性的特征,其在以离子液体为电解质的对称超级电容器中展现了高达3.5 V的电势窗口和255 F g^-1的比容量.本工作为制备新型多功能、高含量杂原子掺杂多孔材料提供了一种通用的方法.

Synthesis of carbon frameworks with N,O and S-lined pores from gallic acid and thiourea for superior CO2 adsorption and supercapacitors

"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(NxOySz)1 carbons with both high content of N/O/S heteroatoms and large specific surface area of up to 1704 m^2 g^-1,which can be efficiently synthesized through a simple additive condensation process using simple gallic acid and thiourea as the building blocks,without subtractive activation.This 1,4-para tri-doped C2(NxOySz)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^-1 at 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 heteroatomdoped porous materials for various applications.