Preparation of highly graphitized porous carbon and its ethane/ethylene separation performance

IF 5.7 3区 材料科学 Q2 Materials Science New Carbon Materials Pub Date : 2024-10-01 DOI:10.1016/S1872-5805(24)60859-0
Ru-shuai Liu, Fan Tang, Xiao-dong Shi, Guang-ping Hao, An-hui Lu
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Abstract

The efficient separation of ethane (C2H6) and ethylene (C2H4) is crucial for the preparation of polymer-grade C2H4, necessitating the development of highly selective and stable C2H6/C2H4 adsorbents. Highly graphitized porous carbon, denoted GC-800, was synthesized by polymerization at room temperature followed by carbonization at 800 °C using phenolic resin as the precursor and FeCl3 as the iron source. Vienna Ab-initio Simulation Package (VASP) calculations confirmed a higher binding energy between C2H6 molecules and graphitized porous carbon surfaces, so that a high degree of graphitization increased the adsorption capacity of porous carbon for C2H6. However, catalytic graphitization using Fe at high temperatures disrupted the microporous structure of the carbon, thereby reducing its ability to separate C2H6/C2H4. By controlling the carbonization temperature, the degree of graphitization and pore structure of the porous carbon could be changed. Raman spectra and XPS spectra showed that the GC-800 had a high degree of graphitization, with a sp2 C content as high as 73%. Low-temperature N2 physical adsorption measurements estimated the specific surface area of GC-800 to be as high as 574 m2·g−1. At 298 K and 1 bar, it had an equilibrium adsorption capacity of 2.16 mmol·g−1 for C2H6, with the C2H6/C2H4 (1:1 and 1:9, v/v) ideal adsorbed solution theory selectivity respectively reaching 2.4 and 3.8, significantly higher than the values of most reported high-performance C2H6 selective adsorbents. Dynamic breakthrough experiments showed that GC-800 could produce high-purity C2H4 in a single step from a mixture of C2H6 and C2H4. Dynamic cycling tests confirmed its good cyclic stability, and that it could efficiently separate C2H6/C2H4 even under humid conditions.
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高石墨化多孔碳的制备及其乙烷/乙烯分离性能
高效分离乙烷(C2H6)和乙烯(C2H4)对于制备聚合物级 C2H4 至关重要,因此需要开发高选择性和高稳定性的 C2H6/C2H4 吸附剂。以酚醛树脂为前驱体,FeCl3 为铁源,在室温下聚合,然后在 800 °C 下碳化,合成了高石墨化多孔碳,命名为 GC-800。维也纳模拟仿真软件包(VASP)的计算证实,C2H6 分子与石墨化多孔碳表面之间的结合能更高,因此高度石墨化提高了多孔碳对 C2H6 的吸附能力。然而,在高温下使用铁进行催化石墨化会破坏碳的微孔结构,从而降低其分离 C2H6/C2H4 的能力。通过控制碳化温度,可以改变多孔碳的石墨化程度和孔隙结构。拉曼光谱和 XPS 光谱显示,GC-800 的石墨化程度很高,sp2 C 含量高达 73%。据低温 N2 物理吸附测量估计,GC-800 的比表面积高达 574 m2-g-1。在 298 K 和 1 bar 条件下,它对 C2H6 的平衡吸附容量为 2.16 mmol-g-1,C2H6/C2H4(1:1 和 1:9,v/v)理想吸附溶液理论选择性分别达到 2.4 和 3.8,明显高于大多数已报道的高性能 C2H6 选择性吸附剂的数值。动态突破实验表明,GC-800 可以一次性从 C2H6 和 C2H4 的混合物中生产出高纯度的 C2H4。动态循环测试证实其具有良好的循环稳定性,即使在潮湿条件下也能有效分离 C2H6/C2H4。
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来源期刊
New Carbon Materials
New Carbon Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
6.10
自引率
8.80%
发文量
3245
审稿时长
5.5 months
期刊介绍: New Carbon Materials is a scholarly journal that publishes original research papers focusing on the physics, chemistry, and technology of organic substances that serve as precursors for creating carbonaceous solids with aromatic or tetrahedral bonding. The scope of materials covered by the journal extends from diamond and graphite to a variety of forms including chars, semicokes, mesophase substances, carbons, carbon fibers, carbynes, fullerenes, and carbon nanotubes. The journal's objective is to showcase the latest research findings and advancements in the areas of formation, structure, properties, behaviors, and technological applications of carbon materials. Additionally, the journal includes papers on the secondary production of new carbon and composite materials, such as carbon-carbon composites, derived from the aforementioned carbons. Research papers on organic substances will be considered for publication only if they have a direct relevance to the resulting carbon materials.
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