Preparation of three-dimensional honeycomb-like material of graphene oxide -carboxylated carbon nanotube-polyethylenepolyamine to adsorb CO2

doi:10.16085/j.issn.1000-6613.2016.11.029

Abstract

Abstract: Using graphene oxide and carboxylated carbon nanotube as base material and gluconic acid β lactone as crosslinking promoter, we prepared a three-dimensional (3D) porous aerogel material functionalized by polyethylenepolyamine (PEPA) with a freeze-drying method. The PEPA loading was adjusted by changing the PEPA dosage. The as-synthesized 3D porous aerogel material were characterized by FTIR, XRD, TG, SEM, XPS, Raman and N₂ adsorption-desorption. The results indicated that PEPA was grafted by an amide bond between PEPA and graphene oxide. The 3D porous material had a honeycomb like-appearance. The specific surface area, pore volume and average pore size were decreased with increasing PEPA loading. The adsorption of CO₂ on the 3D honeycomb-like material was based on a mechanism of chemisorption. At 200kPa and 328K, the CO₂adsorption capacity on the 3D porous material with a PEPA content of 55.8% reached up to 3.9mmol/g, which was 9.8 times to that on the aerogel without PEPA loading. The results showed that crosslinking polyethylenepolyamine with graphene oxide sheet and carboxylated carbon nanotube to prepare 3D porous aerogel material effectively improved the CO₂ adsorption capacity.

Key words: nanomaterials, carbon dioxide, gels, adsorption

摘要： 以氧化石墨烯-羧基碳纳米管水溶液为原料，葡萄糖酸β内酯为交联促进剂，通过冷冻干燥法制得负载有多乙烯多胺的氧化石墨烯-羧基碳纳米管三维多孔气凝胶。通过在制备过程中改变多乙烯多胺的加入量可以调节其负载量。FTIR、XRD、TG、SEM、XPS、Raman、N₂吸脱附等测试表征发现：多乙烯多胺通过酰胺键与基体连接，所得材料呈蜂窝状，且比表面积、孔容和平均孔径随胺类负载量的增加而逐渐降低，引入多乙烯多胺后的气凝胶材料通过化学作用实现CO₂吸附。在200kPa、328K下，多乙烯多胺含量为55.8%的改性吸附剂的CO₂吸附量可达3.9mmol/g，为相同条件下未改性吸附剂的9.8倍。结果表明，将多乙烯多胺、氧化石墨烯和羧基碳纳米管制备成三维蜂窝状多孔材料能有效提高CO₂吸附性能。

关键词: 纳米材料, 二氧化碳, 凝胶, 吸附

CLC Number:

TQ424.29

HU Hangbiao, ZHANG Tao, CUI Zheng, TANG Shengwei. Preparation of three-dimensional honeycomb-like material of graphene oxide -carboxylated carbon nanotube-polyethylenepolyamine to adsorb CO₂[J]. Chemical Industry and Engineering Progress, 2016, 35(11): 3576-3584.

胡航标, 张涛, 崔征, 唐盛伟. 氧化石墨烯-羧基碳纳米管-多乙烯多胺三维蜂窝状材料吸附CO₂[J]. 化工进展, 2016, 35(11): 3576-3584.

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Preparation of three-dimensional honeycomb-like material of graphene oxide -carboxylated carbon nanotube-polyethylenepolyamine to adsorb CO₂

氧化石墨烯-羧基碳纳米管-多乙烯多胺三维蜂窝状材料吸附CO₂

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