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(NxOySz)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(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−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.
摘要
“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 m2 g−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.
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Acknowledgements
The Max Planck Society is gratefully acknowledged for financial support. We thank Regina Rothe for technical assistance. Tian Z sincerely acknowledges the financial support provided by Zhengzhou University and the National Natural Science Foundation of China (51873198).
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Author contributions Tian Z and Antonietti M conceived the idea and cowrote the paper. Tian Z and Lai F designed and performed the experiments and analyzed the results. Tobias H performed the HRTEM tests. All the authors discussed the results and commented on the manuscript.
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Zhihong Tian obtained her PhD degree in applied chemistry at Zhengzhou University in 2018. She has been working in Zhengzhou University since June 2018. Currently, she is a visiting postdoctor in Professor Markus Antonietti’s Group at Max Planck Institute of Colloids and Interfaces (MPICI). Her research interests lie in the design and synthesis of porous polymer and carbon materials for gas separation, energy storage and conversion.
Markus Antonietti is a professor at MPICI. He studied chemistry in Mainz, where he also received his PhD in 1985. His habilitation on nanogels in 1990 fueled his enthusiasm for complex nanostructures based on polymers and carbon. After a professorship at the University of Marburg, he was appointed director for the Department of Colloid Chemistry at MPICI in 1993. His work deals with modern materials chemistry, energy materials, and sustainability issues within those topics.
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Synthesis of carbon frameworks with N, O and S-lined pores from gallic acid and thiourea for superior CO2 adsorption and supercapacitors
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Tian, Z., Lai, F., Heil, T. et al. Synthesis of carbon frameworks with N, O and S-lined pores from gallic acid and thiourea for superior CO2 adsorption and supercapacitors. Sci. China Mater. 63, 748–757 (2020). https://doi.org/10.1007/s40843-019-1254-9
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DOI: https://doi.org/10.1007/s40843-019-1254-9