摘要
针对有机聚合物材料对CO_(2)的吸附量和吸附选择性不能兼得的问题,由三(4-氰胺基苯基)胺和四(4-氰胺基苯基)甲烷设计合成了仲胺桥联共价三嗪聚合物NB-CTP-1和NB-CTP-2,通过FTIR、TGA、XRD、SEM、TEM和全自动物理吸附分析仪对制备的样品进行了结构和形貌表征。在1.01×10^(5) Pa、273K条件下,NB-CTP-1和NB-CTP-2的CO_(2)吸附量分别为3.04和3.23 mmol/g。依据亨利定律法和IAST法分别对两种材料在1.01×10^(5) Pa、273K条件下的吸附选择性进行计算,其中,NB-CTP-1的CO_(2)/N_(2)吸附选择性高达113 (亨利定律法)和143(IAST法),而NB-CTP-2也能达到75(亨利定律法)和89(IAST法)。此外,通过Clausius-Clapeyron方程计算得出NB-CTP-1和NB-CTP-2的极限吸附热分别为35.3和37.6 kJ/mol,表明其与CO_(2)存在较强的偶极-四极相互作用,有利于提升吸附选择性。
Nitrogen-bridged covalent triazine polymers NB-CTP-1 and NB-CTP-2 were designed and synthesized from tris(4-cyanamidophenyl)amine and tetrakis(4-cyanamidophenyl)methane to address the issue of trade-off between CO_(2) adsorption capacity and CO_(2)/N_(2) adsorption selectivity among the well-established organic polymers. The structure and morphology features of the prepared samples were characterized by means of FTIR, TGA, XRD, SEM, TEM and automatic physical adsorption analyzer. The NB-CTP materials showed good CO_(2) adsorption capacities(3.04 mmol/g for NB-CTP-1, 3.23 mmol/g for NB-CTP-2) under 1.01×10^(5) Pa and 273 K conditions. Based on the reversible adsorption-desorption isotherms at 1.01×10^(5) Pa and 273 K, CO_(2)/N_(2) selectivity for NB-CTP-1 was obtained as high as 113(Henry’s law) and 143(IAST), whereas for NB-CTP-2, it was 75(Henry’s law) and 89(IAST). In addition,the enthalpy of adsorption at zero coverage for NB-CTP-1(35.3 kJ/mol) and NB-CTP-2(37.6 kJ/mol)were calculated using the Vant Hoff equation based on Virial equation, revealing the strong dipole-quadrupole interactions between these materials and CO_(2), which could enhance the CO_(2)/N_(2) adsorption selectivity.
作者
沙芯如
张金菊
刘安华
SHA Xinru;ZHANG Jinju;LIU Anhua(State Key Laboratory of Fine Chemicals,School of Chemical Engineering,Dalian University of Technology,Dalian 116023,Liaoning,China)
出处
《精细化工》
EI
CAS
CSCD
北大核心
2021年第10期1988-1995,共8页
Fine Chemicals
基金
大连理工大学基本科研业务费项目(DUT20LK17)。
关键词
共价三嗪聚合物
CO_(2)
捕集
吸附选择性
吸附热
碳中和
碳达峰
功能材料
covalent triazine polymer
carbon dioxide
capture
adsorption selectivity
enthalpy of adsorption
carbon neutrality
peak carbon dioxide emissions
functional materials
