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提高多孔碳杂原子掺杂水平以获得优异 CO 捕集和分离性能的有效方法。

Effective Approach for Increasing the Heteroatom Doping Levels of Porous Carbons for Superior CO Capture and Separation Performance.

机构信息

Department of Mechanical and Nuclear Engineering, Virginia Commonwealth University , 401 West Main Street, Richmond, Virginia 23284-2006, United States.

Department of Nuclear and Radiation Engineering, Alexandria University , Alexandria 21544, Egypt.

出版信息

ACS Appl Mater Interfaces. 2017 Oct 18;9(41):35802-35810. doi: 10.1021/acsami.7b09989. Epub 2017 Oct 9.

DOI:10.1021/acsami.7b09989
PMID:28956436
Abstract

Development of efficient sorbents for carbon dioxide (CO) capture from flue gas or its removal from natural gas and landfill gas is very important for environmental protection. A new series of heteroatom-doped porous carbon was synthesized directly from pyrazole/KOH by thermolysis. The resulting pyrazole-derived carbons (PYDCs) are highly doped with nitrogen (14.9-15.5 wt %) as a result of the high nitrogen-to-carbon ratio in pyrazole (43 wt %) and also have a high oxygen content (16.4-18.4 wt %). PYDCs have a high surface area (SA = 1266-2013 m g), high CO Q (33.2-37.1 kJ mol), and a combination of mesoporous and microporous pores. PYDCs exhibit significantly high CO uptakes that reach 2.15 and 6.06 mmol g at 0.15 and 1 bar, respectively, at 298 K. At 273 K, the CO uptake improves to 3.7 and 8.59 mmol g at 0.15 and 1 bar, respectively. The reported porous carbons also show significantly high adsorption selectivity for CO/N (128) and CO/CH (13.4) according to ideal adsorbed solution theory calculations at 298 K. Gas breakthrough studies of CO/N (10:90) at 298 K showed that PYDCs display excellent separation properties. The ability to tailor the physical properties of PYDCs as well as their chemical composition provides an effective strategy for designing efficient CO sorbents.

摘要

开发高效的二氧化碳(CO)捕获吸附剂,用于从烟道气中捕集 CO,或从天然气和垃圾填埋气中脱除 CO,对于环境保护非常重要。本文通过热解法直接从吡唑/ KOH 合成了一系列杂原子掺杂的多孔碳。由于吡唑(43wt%)中氮与碳的比例很高,所得到的吡唑衍生碳(PYDC)中氮含量高达 14.9-15.5wt%,同时氧含量也很高(16.4-18.4wt%)。PYDC 的比表面积(SA=1266-2013m2/g)高,CO 吸附量 Q 高(33.2-37.1kJ/mol),介孔和微孔并存。在 298K 时,PYDC 在 0.15 和 1 巴下的 CO 吸附量分别高达 2.15 和 6.06mmol/g。在 273K 时,CO 吸附量分别提高到 3.7 和 8.59mmol/g。根据 298K 时理想吸附溶液理论计算,所报道的多孔碳对 CO/N(128)和 CO/CH(13.4)的吸附选择性也非常高。在 298K 下对 CO/N(10:90)的气体穿透研究表明,PYDC 显示出优异的分离性能。调节 PYDC 物理性能和化学组成的能力为设计高效 CO 吸附剂提供了一种有效的策略。

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