吲哚基多孔有机聚合物对碘蒸气的吸附性能  

Iodine vapor adsorption performance of indole-based porous organic polymers

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作  者:于静文 李忠[1,2] 武蒙蒙[1,2] 冯宇[1,2] 米杰[1,2] YU Jingwen;LI Zhong;WU Mengmeng;FENG Yu;MI Jie(State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Key Laboratory of Coal Science and Technology,Ministry of Education,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Lu’an Chemical Group Co.,Ltd.,Changzhi 046204,Shanxi,China)

机构地区:[1]太原理工大学省部共建煤基能源清洁高效利用国家重点实验室,山西太原030024 [2]太原理工大学煤科学与技术教育部重点实验室,山西太原030024 [3]潞安化工集团有限公司,山西长治046204

出  处:《低碳化学与化工》2025年第4期90-97,106,共9页Low-Carbon Chemistry and Chemical Engineering

基  金:国家自然科学基金(21978188)。

摘  要:研发高效放射性碘吸附材料对核废料处理及核能安全利用具有重要意义。分别以2-苯基吲哚(2-PhIn)和1-甲基-2-苯基吲哚(1-Me-2-PhIn)为构筑单元,甲缩醛(FDA)为外交联剂,在无水FeCl_(3)催化作用下通过Friedel-Crafts烷基化反应合成了两种多孔有机聚合物,研究了聚合物的碘蒸气吸附性能及构效关系。结果表明,甲基空间位阻效应对聚合过程产生了不利影响,导致聚合物孔结构较差。聚合物碘吸附性能受吸附位点和孔结构双重影响。1-Me-2-PhIn-P碘吸附量更高(2.99 g/g),优于商业活性炭。在首次碘蒸气吸附过程中,主要以化学吸附作用为主,I2与富π电子聚合物骨架通过路易斯酸/碱相互作用转变为聚碘阴离子(I3-和I5-),且较大的平均孔径有助于客体碘物种富集。此外,吸附碘蒸气后的1-Me-2-PhIn-P可在125℃下再生,经5次循环后碘吸附量和吸附效率仍可分别保持在1.81 g/g和60.5%,物理吸附在多次循环实验中发挥主导作用。本研究可为气态放射性碘吸附材料开发提供新借鉴。The development of highly efficient radioactive iodine adsorption materials is of great significance for the disposal of nuclear waste and the safe utilization of nuclear energy.Two kinds of porous organic polymers were synthesized via Friedel-Crafts alkylation reaction using 2-phenylindole(2-PhIn)and 1-methyl-2-phenylindole(1-Me-2-PhIn)as the building units,formaldehyde dimethyl acetal(FDA)as the external cross-linker and anhydrous FeCl_(3) as the catalyst.The iodine vapor adsorption properties and structure-activity relationships of the polymers were investigated.It is found that the steric hindrance effect of methyl group has a negative impact on the polymerization process,resulting in polymers with poor pore texture.The iodine adsorption properties of polymers are influenced by both the adsorption sites and the pore structures.1-Me-2-PhIn-P exhibits a higher iodine adsorption capacity(2.99 g/g),which is superior to commercial activated carbon.During the initial iodine vapor adsorption process,chemisorption plays a dominant role,where I2 interacts with theπ-electron-rich polymer framework through Lewis acid/base interactions to form polyiodide anions(I-3 and I-5).Furthermore,the larger average pore size facilitates the enrichment of guest iodine species.Additionally,1-Me-2-PhIn-P adsorbed with iodine vapor can be regenerated at 125℃.After 5 cycles,the iodine adsorption capacity and adsorption efficiency can still be maintained at 1.81 g/g and 60.5%,respectively.Physisorption plays a major role in the cycling experiments.This research can offer new references for the development of gaseous radioactive iodine adsorption materials.

关 键 词:吲哚 多孔有机聚合物 碘蒸气 吸附性能 

分 类 号:TQ424.3[化学工程] X591[环境科学与工程—环境工程]

 

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