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氮硫共掺杂微孔活性炭大球用于 CO2 捕集。

Nitrogen and sulfur Co-doped microporous activated carbon macro-spheres for CO capture.

机构信息

Institute of Coal Chemistry, Chinese Academy of Sciences, 27 South Taoyuan Road, Taiyuan 030001, Shanxi, PR China; University of Chinese Academy of Sciences, 19A Yuquan Road, Beijing 100049, PR China.

Institute of Coal Chemistry, Chinese Academy of Sciences, 27 South Taoyuan Road, Taiyuan 030001, Shanxi, PR China.

出版信息

J Colloid Interface Sci. 2018 Sep 15;526:174-183. doi: 10.1016/j.jcis.2018.04.101. Epub 2018 Apr 27.

DOI:10.1016/j.jcis.2018.04.101
PMID:29734086
Abstract

Millimeter-sized nitrogen and sulfur co-doped microporous activated carbon spheres (NSCSs) were first synthesized from poly(styrene-vinylimidazole-divinylbenzene) resin spheres through concentrated HSO sulfonation, carbonization and KOH activation. Styrene (ST) and N-vinylimidazole (VIM) were carbon and nitrogen sources, while the sulfonic acid functional groups introduced by the simple concentrated sulfuric acid sulfonation worked simultaneously as cross-linking agent and sulfur source during the following thermal treatments. It was found that the surface chemistries, textural structures, and CO adsorption performances of the NSCSs were significantly affected by the addition of VIM. The NSCS-4-700 sample with a molar ratio of ST: VIM = 1: 0.75 showed the best CO uptake at different temperatures and pressures. An exhaustive adsorption evaluation indicated that CO sorption at low pressures originated from the synergistic effect of surface chemistry and micropores below 8.04 Å, while at the moderate pressure of 8.0 bar, CO uptake was dominated by the volume of micropores. The thermodynamics suggested the exothermic and orderly nature of the adsorption process, which was dominated by a physisorption mechanism. The high CO adsorption capacity, fast kinetic adsorption rate, and great regeneration stability of the nitrogen and sulfur co-doped activated carbon spheres indicated that the as-prepared carbon adsorbents were good candidates for large-scale CO capture.

摘要

首次通过浓 HSO4 磺化、碳化和 KOH 活化,从聚苯乙烯-乙烯基咪唑-二乙烯基苯树脂球体制备出毫米级的氮硫共掺杂微孔活性炭球(NSCSs)。苯乙烯(ST)和 N-乙烯基咪唑(VIM)分别作为碳源和氮源,而简单的浓硫酸磺化引入的磺酸官能团在后续的热处理过程中同时作为交联剂和硫源。研究发现,VIM 的添加显著影响了 NSCSs 的表面化学、结构和 CO 吸附性能。在不同温度和压力下,ST:VIM摩尔比为 1:0.75 的 NSCS-4-700 样品表现出最佳的 CO 吸附量。详尽的吸附评估表明,低压下的 CO 吸附源于表面化学和 8.04 Å 以下微孔的协同作用,而在 8.0 bar 的中等压力下,CO 吸附主要由微孔体积决定。热力学表明吸附过程是放热和有序的,主要由物理吸附机制控制。氮硫共掺杂活性炭球具有高的 CO 吸附容量、快速的动力学吸附速率和良好的再生稳定性,表明所制备的碳吸附剂是大规模 CO 捕获的良好候选材料。

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