期刊
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
卷 9, 期 2, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.jece.2021.105046
关键词
Ultramicropore-enriched N-doped carbon; Polymer network; Self-decomposition; Pore formation; Surface polarity; CO2 capture
资金
- National Natural Science Foundation of China [21908092, U19B2001, 21878159]
- Foundation from State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University [ZK201712]
N-doped porous carbons with ultramicropore enrichment were synthesized from polyethyleneimine-based polymer network, showing excellent CO2 adsorption performance. Fine-tuning of structure and nitrogen content was achieved by adjusting carbonization temperature and activator amount.
N-doped porous carbons have been regarded as competitive candidates for CO2 adsorption by virtue of tunable micropores and basic nitrogen sites. Herein, we synthesized the ultramicropore-enriched N-doped carbon by pyrolysis of polyethyleneimine-based polymer network which was formed by nucleophilic substitution reaction of polyethyleneimine and p-dichloroxylene. The precursor with evenly anchored amine groups on the surface and interior could not only serve as pore-forming agent by self-decomposition, but also generate abundant nitrogen sites to enhance the surface polarity. By adjusting carbonization temperatures (500, 600, 700 and 800 degrees;C) and amounts of KOH activator, the texture properties and nitrogen contents of the N-doped porous carbons (denoted as CPDs) were tuned finely. Impressively, the CPD-600 pyrolyzed at 600 degrees C possessed large surface area (1638 m(2)/g), narrow-distributed ultramicropores (d < 0.7 nm) and high nitrogen content (6.16 wt%). The sufficient nitrogen species (especially pyrrolic-N) as the basic CO2-philic sites could strengthen the affinity of polar surfaces toward CO2 molecules. Moreover, the well-developed ultramiropores offered restricted spaces that could capture CO2 by superposition effect of Van der Waals' force. These advantages endowed CPD-600 with high-performance of CO2 uptake (4.92 mmol/g), CO2/N-2 (15/85, v/v) selectivity (31) and regenerability at 298 K and 1 bar. The rational design of polymer-derived porous carbons with tailoring structural and functional properties could be applied not only to CO2 capture from gas mixtures but also to other advanced fields.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据