富氮共价有机框架材料的合成及其碘吸附性能研究
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摘要
放射性碘因其易挥发性、生物相容性以及高迁移率等性质成为气体放射性核废物中极为重要的污染物,一旦泄露到环境中将会产生巨大的危害.因此,高效的碘吸附材料的研究与开发意义重大.共价有机框架(covalent organic framework, COF)材料是一类新兴的结晶多孔聚合物材料,具有高度灵活的分子可设计性和孔道结构可调控性.富氮结构和富电子π-π共轭体系的COF材料能够为碘的吸附提供有效结合位点,是良好的吸附剂备选材料.本文选用高含氮化合物2,4,6-三对甲酰苯氧基-1,3,5-三嗪(TPT-CHO)为单体,通过醛胺缩合反应合成了富氮的新型COF材料——TPT-DMB COF.吸附实验表明,制备产物对气态碘具有大容量、高效和可逆的吸附特性,最大吸附容量可达5150 mgg~(-1),高于绝大多数已报道的吸附剂材料.这些特性使该材料在放射性碘的富集与分离领域具有极大的应用前景.
Radioactive iodine is a very important pollutant among the radioactive nuclear waste gases because of its easy volatile, high biocompatibility and mobility. Once leaking into the environment, it will bring huge harm to ecology environment. Therefore, the development of high efficient adsorption materials for iodine is of great significance.Covalent organic framework(COF) is a kind of novel porous crystal polymer with highly flexible molecular designability and regulable channel structure. COF containing nitrogen-rich structure and electron-rich π-π conjugated system can provide effective binding sites for iodine adsorption, and is a potential adsorption material. In this paper, a nitrogen-rich monomer, 2,4,6-tris(4-formylphenoxy)-1,3,5-triazine(TPT-CHO) was chosen to construct a new nitrogenrich COF(TPT-DMB COF) through the condensation of aldehyde and amine. It was found by adsorption experiments that TPT-DMB COF showed large capacity, high efficiency and reversible adsorption properties for volatile iodine. The maximum adsorption capacity can reach 5150 mgg~(-1), higher than that of most reported adsorption materials. The advantages endow the material with great application prospects in the field of enrichment and separation of radioactive iodine.
Radioactive iodine is a very important pollutant among the radioactive nuclear waste gases because of its easy volatile, high biocompatibility and mobility. Once leaking into the environment, it will bring huge harm to ecology environment. Therefore, the development of high efficient adsorption materials for iodine is of great significance.Covalent organic framework(COF) is a kind of novel porous crystal polymer with highly flexible molecular designability and regulable channel structure. COF containing nitrogen-rich structure and electron-rich π-π conjugated system can provide effective binding sites for iodine adsorption, and is a potential adsorption material. In this paper, a nitrogen-rich monomer, 2,4,6-tris(4-formylphenoxy)-1,3,5-triazine(TPT-CHO) was chosen to construct a new nitrogenrich COF(TPT-DMB COF) through the condensation of aldehyde and amine. It was found by adsorption experiments that TPT-DMB COF showed large capacity, high efficiency and reversible adsorption properties for volatile iodine. The maximum adsorption capacity can reach 5150 mgg~(-1), higher than that of most reported adsorption materials. The advantages endow the material with great application prospects in the field of enrichment and separation of radioactive iodine.
引文
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2 Ewing RC.Nat Mater,2015,14:252-257
3 Pang H,Wang X,Yao W,Yu S,Wang X.Sci Sin Chim,2018,48:58-73
4 Verde G.J Fundam Appl Sci,2017,9:1211-1224
5 Steinhauser G,Brandl A,Johnson TE.Sci Total Environ,2014,470-471:800-817
6 Haefner DR.Tranter TJ.Methods of Gas Phase Capture of Iodine from Fuel Reprocessing Off-Gas:A Literature Survey.Idaho Falls:Idaho National Laboratory,2007
7 C?téAP,Benin AI,Ockwig NW,O’Keeffe M,Matzger AJ,Yaghi OM.Science,2005,310:1166-1170
8 Chen X,Huang N,Gao J,Xu H,Xu F,Jiang D.Chem Commun,2014,50:6161-6163
9 Sun B,Mo Y,Wang L,Yue J,Wang D.Sci Sin Chim,2016,46:994-1006(in Chinese)[孙兵,莫依萍,汪利梅,岳婕妤,王栋.中国科学:化学,2016,46:994-1006]
10 Yin ZJ,Xu SQ,Zhan TG,Qi QY,Wu ZQ,Zhao X.Chem Commun,2017,53:7266-7269
11 Qian X,Zhu ZQ,Sun HX,Ren F,Mu P,Liang W,Chen L,Li A.ACS Appl Mater Interfaces,2016,8:21063-21069
12 Yan Z,Yuan Y,Tian Y,Zhang D,Zhu G.Angew Chem Int Ed,2015,54:12733-12737
13 Ma H,Chen JJ,Tan L,Bu JH,Zhu Y,Tan B,Zhang C.ACS Macro Lett,2016,5:1039-1043
14 Chapman KW,Chupas PJ,Nenoff TM.J Am Chem Soc,2010,132:8897-8899
15 Katsoulidis AP,He J,Kanatzidis MG.Chem Mater,2012,24:1937-1943
16 Geng T,Zhu Z,Zhang W,Wang Y.J Mater Chem A,2017,5:7612-7617
17 Liao Y,Weber J,Mills BM,Ren Z,Faul CFJ.Macromolecules,2016,49:6322-6333
18 Zhu Y,Ji YJ,Wang DG,Zhang Y,Tang H,Jia XR,Song M,Yu G,Kuang GC.J Mater Chem A,2017,5:6622-6629
19 Chen Y,Sun H,Yang R,Wang T,Pei C,Xiang Z,Zhu Z,Liang W,Li A,Deng W.J Mater Chem A,2015,3:87-91
20 Dang QQ,Wang XM,Zhan YF,Zhang XM.Polym Chem,2016,7:643-647
21 A S,Zhang Y,Li Z,Xia H,Xue M,Liu X,Mu Y.Chem Commun,2014,50:8495-8498
22 Sava DF,Rodriguez MA,Chapman KW,Chupas PJ,Greathouse JA,Crozier PS,Nenoff TM.J Am Chem Soc,2011,133:12398-12401
23 Sava DF,Chapman KW,Rodriguez MA,Greathouse JA,Crozier PS,Zhao H,Chupas PJ,Nenoff TM.Chem Mater,2013,25:2591-2596
24 Wang C,Wang Y,Ge R,Song X,Xing X,Jiang Q,Lu H,Hao C,Guo X,Gao Y,Jiang D.Chem Eur J,2018,24:585-589
25 Pei C,Ben T,Xu S,Qiu S.J Mater Chem A,2014,2:7179-7187
26 Svensson PH,Kloo L.Chem Rev,2003,103:1649-1684