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聚丙烯腈树脂基固态胺吸附剂的制备及其对CO2吸附性能研究
Synthesis and CO2 Adsorption Behavior of Amine-functionalized Porous Polyacrylonitrile Resin
- 高分子学报 2018年0卷第7期 页码：886-892
- 作者机构：
中山大学化学学院 广州 512075
- 作者简介：
E-mail: cescsx@mail.sysu.edu.cn Shuixia Chen, E-mail: cescsx@mail.sysu.edu.cn
- 基金信息：国家自然基金项目(基金号 51473187)和广东省科技计划项目(项目号 2016A010103013)资助()
DOI：10.11777/j.issn1000-3304.2018.17332
中图分类号：纸质出版日期：2018-7，
收稿日期：2017-12-18，
修回日期：2018-1-6，
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刘风雷, 陈水挟, 符文皓. 聚丙烯腈树脂基固态胺吸附剂的制备及其对CO2吸附性能研究[J]. 高分子学报, 2018,0(7):886-892.
Feng-lei Liu, Shui-xia Chen, Wen-hao Fu. Synthesis and CO2 Adsorption Behavior of Amine-functionalized Porous Polyacrylonitrile Resin[J]. Acta Polymerica Sinica, 2018,0(7):886-892.
刘风雷, 陈水挟, 符文皓. 聚丙烯腈树脂基固态胺吸附剂的制备及其对CO2吸附性能研究[J]. 高分子学报, 2018,0(7):886-892. DOI： 10.11777/j.issn1000-3304.2018.17332.
Feng-lei Liu, Shui-xia Chen, Wen-hao Fu. Synthesis and CO2 Adsorption Behavior of Amine-functionalized Porous Polyacrylonitrile Resin[J]. Acta Polymerica Sinica, 2018,0(7):886-892. DOI： 10.11777/j.issn1000-3304.2018.17332.
摘要
以丙烯腈(AN)为单体，二乙烯苯(DVB)为交联剂，采用悬浮聚合法制备了多孔聚丙烯腈聚合物(PAN)，进一步通过胺化反应制备了含有较高密度胺基的固态胺吸附材料. 利用N
2
吸附-脱附等温线、扫描电子显微镜(SEM)、热重分析(TG)等方法表征了吸附材料的结构和形貌. 研究了有机胺化试剂类型对所制备的材料结构的影响，以及吸附温度、湿度等对其CO
2
吸附性能的影响. 研究结果表明，当吸附温度为25 °C、流速为30 mL/min、CO
2
浓度为10%、有机胺为四乙烯五胺(TEPA)时，固态胺吸附材料PAN-TEPA对CO
2
的吸附量可达1.87 mmol/g. 水的存在能显著提高PAN-TEPA的吸附量，饱和水蒸气下，其对CO
2
的平衡吸附量为2.97 mmol/g. 动力学研究发现，Avrami模型能很好地拟合PAN-TEPA在不同温度下的吸附过程，揭示PAN-TEPA对CO
2
的吸附过程是物理吸附和化学吸附共同作用的效果. 经过10次循环再生吸附后，PAN-TEPA的吸附量仍可以达到初始吸附量的98%. 上述研究结果表明，PAN-TEPA对CO
2
具有良好的吸附性能和稳定的再生性能，其在CO
2
的捕集方面具有重要的应用前景.
Abstract
The objective of this study was to develop a novel solid amine adsorbent using porous polyacrylonitrile resin instead of mesoporous silica as support for CO
2
adsorption from flue gas. This solid amine adsorbent was prepared by a suspension polymerization of divinylbenzene (DVB) with acrylonitrile (AN)
followed by aminating with tetraethylenepentamine (TEPA). Scanning electronic microscope
nitrogen adsorption-desorption isotherms at 77 K
and thermogravimetry (TG) were employed to characterize the surface structure
porosity
and thermal stability of the solid amine adsorbent. Factors that could determine the CO
2
adsorption performance of the solid amine adsorbent
such as amine species
adsorption temperature and moisture
were investigated. The experimental results showed that the maximum adsorption capacity of CO
2
(1.87 mmol/g) wasachieved at 25 °C with CO
2
concentration of 10 vol%
the flow rate of 30 mL/min and TEPA as the organic amine. The solid amine adsorbent modified with TEPA (PAN-TEPA)
a longer chain amine among all amines used
showed superior amine efficiency and CO
2
adsorption capacity to the other two amine species with shorter chains. CO
2
adsorption capacity decreased obviously as the adsorption temperature increased
because the reaction between CO
2
and amine groups was an exothermic reaction. The presence of water could significantly improve CO
2
amount adsorbed on the adsorbent by promoting the chemical adsorption of CO
2
on PAN-TEPA. A higher equilibrium adsorption capacity (2.97 mmol/g) was achieved in the presence of moisture. Meanwhile
the kinetics study found that Avrami kinetic model was more fitted to accurately describe CO
2
adsorption than the Pseudo-first and Pseudo-second order models
indicating that both physical adsorption and chemical adsorption were involved in CO
2
adsorption. Moreover
this solid amine adsorbent could be regenerated with nitrogen stream at 75 °C
and it kept stable CO
2
adsorption capacity after ten cycles of adsorption-desorption. All these features indicated that the amine-functionalized porous polyacrylonitrile resin has a high potential for CO
2
capture and separation from flue gas.
关键词
CO2吸附多孔性聚合物动力学
Keywords
CO2AdsorptionPorous polymerKinetics
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