选择性吸附Pt(Ⅳ)的杯芳烃纤维制备及其吸附动力学
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摘要
为制备含杯芳烃的新型选择性吸附纤维,首先通过酰胺化和静电纺丝技术制备杯芳烃聚酰胺酸(CPAA)纤维,再将CPAA纤维通过热亚胺化制备得到杯芳烃聚酰亚胺(CPI)纤维,借助红外光谱仪、扫描电子显微镜、热重分析仪分析了纤维的结构和性能,并采用吸附实验研究了纤维的吸附选择性及动力学。结果表明:杯芳烃已引入纤维中,对比CPAA纤维,CPI纤维具有直径更小,主链分解温度更高的优点;CPI纤维可从Pt(Ⅳ)、Ag(Ⅰ)混合溶液中选择性吸附Pt(Ⅳ),溶液pH值为7时吸附量最大,达28 mg/g;CPI纤维吸附Pt(Ⅳ)符合一级动力学特征,20℃时吸附速率常数为0.003 9 min~(-1),且吸附速率常数随温度升高而增大;CPI纤维易吸附Pt(Ⅳ),吸附所克服的活化能较低,仅为12.24 kJ/mol。
In order to prepare novel selective adsorption fibers containing calixarene, calixarene polyamide acid(CPAA) fibers were firstly prepared by amidating and electrospinning. Subsequently, the calixarene polyimide(CPI) fibers were obtained by thermal imidization of the CPAA fibers. The CPI and CPAA fibers were characterized by Fourier transform infrared spectrometer, scanning electron microscope and thermogravimetric analysis. The adsorption selectivity and adsorption kinetics of the CPI fibers were also investigated. The results show that calixarene is successfully incorporated into the CPAA and CPI fibers. The CPI fibers possess smaller diameter and higher thermal degradation temperatur by comparison with the CPAA fibers. Only the CPI fibers can adsorb Pt(Ⅳ) selectively from the mixture of Pt(Ⅳ) and Ag(I). The maximum Pt(Ⅳ) absorption capacity of CPI fibers is 28 mg/g at pH 7, and its adsorption behavior fits well with the first-order adsorption kinetics model. The adsorption rate constant is 0.003 9 min~(-1) at 20 ℃ and increases with the elevating adsorption temperature. The required activation energy for adsorption is only 12.24 kJ/mol, which indicates the CPI fibers adsorbing Pt(Ⅳ) is easy to occur.
In order to prepare novel selective adsorption fibers containing calixarene, calixarene polyamide acid(CPAA) fibers were firstly prepared by amidating and electrospinning. Subsequently, the calixarene polyimide(CPI) fibers were obtained by thermal imidization of the CPAA fibers. The CPI and CPAA fibers were characterized by Fourier transform infrared spectrometer, scanning electron microscope and thermogravimetric analysis. The adsorption selectivity and adsorption kinetics of the CPI fibers were also investigated. The results show that calixarene is successfully incorporated into the CPAA and CPI fibers. The CPI fibers possess smaller diameter and higher thermal degradation temperatur by comparison with the CPAA fibers. Only the CPI fibers can adsorb Pt(Ⅳ) selectively from the mixture of Pt(Ⅳ) and Ag(I). The maximum Pt(Ⅳ) absorption capacity of CPI fibers is 28 mg/g at pH 7, and its adsorption behavior fits well with the first-order adsorption kinetics model. The adsorption rate constant is 0.003 9 min~(-1) at 20 ℃ and increases with the elevating adsorption temperature. The required activation energy for adsorption is only 12.24 kJ/mol, which indicates the CPI fibers adsorbing Pt(Ⅳ) is easy to occur.
引文
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[23] 凤权, 武丁胜, 桓珊,等. AOPAN/RC纳米纤维膜的制备及对金属离子吸附性能[J]. 高分子材料科学与工程, 2017, 33(8):140-144.FENG Quan, WU Dingsheng, HUAN Shan, et al. Preparation and metal ion adsorption properties of AOPAN/RC nanofibrous membrane[J].Polymer Materials Science and Engineering, 2017, 33(8):140-144.
[2] ERMAKOVA T G, SHAULINA L P, KUZNETSOVA N P, et al. Sorption recovery of noble metal ions with a copolymer of 1-vinyl-1,2,4-triazole with acrylo-nitrile [J]. Russian Journal of Applied Chemistry, 2012, 85(8):1289-1295.
[3] BRAY D J, CLEGG J K, WENZEL M, et al. Selective solvent extraction of silver(I) by tris-pyridyl tripodal ligands and X-ray structure of a silver(I) coordination polymer incorporating one such ligand [J]. Australian Journal of Chemistry, 2015, 68(4):549-554.
[4] ALI S A, KAZI I W, ULLAH N. New chelating ion-exchange resin synthesized via the cyclopolymerization protocol and its uptake performance for metal ion removal[J]. Industrial and Engineering Chemistry Research, 2015, 54 (40): 9689-9698.
[5] RIVAS B L, POOLEY S A, PEREIRA E, et al. Water-soluble polymer materials as complexing reagents for the separation of metal ions using membrane filtration[J]. Polymers for Advanced Technologies, 2006, 17(11/12):671-684.
[6] 凤权,王清清,魏取福,等. Cd2+-PVA/PA6金属配合纳米纤维的制备及反应动力学分析[J]. 纺织学报, 2012, 33(3): 5-8.FENG Quan, WANG Qingqing, WEI Qufu, et al. Preparation of Cd2+-PVA/PA6 metal chelated nanofibers and analysis of reaction kinetics[J]. Journal of Textile Research, 2012, 33(3): 5-8.
[7] DENG S, ZHANG G S, WANG X, et al. Preparation and performance of polyacrylonitrile fiber functionalized with iminodiacetic acid under microwave irradiation for adsorption of Cu(II) and Hg(II) [J]. Chemical Engineering Journal, 2015, 276:349-357.
[8] FONG H, CHUN I, RENEKER D H. Beaded nanofibers formed during electrospinning [J]. Polymer, 1999, 40(16):4585-4592.
[9] CHASE G G, VARABHAS J S, RENEKER D H. New methods to electrospin nanofibers [J]. Journal of Engineered Fibers and Fabrics, 2011, 6(3):32-38.
[10] TAO X C, LI L, HE J X. Synthesis of bis-substituted calix[4]arenes and mechanism of substituents effect on K+ and Hg2+ ions transports through liquid mem-brane[J]. Journal of Donghua University (English Edition), 2011, 28(6): 621-623.
[11] TAO X C, LI L.Synthesis and transport of K+ ions of mono-substituted calix[4]arenes[J]. Advanced Materials Research, 2012, 441: 392-397.
[12] TAO X C, HE J X. Synthesis of calix [4] arene thia derivative and extraction effect of substituents on mercury (Ⅱ) and lead (Ⅱ) [J]. Journal of Donghua University (English Edition), 2017, 34(1):49-52.
[13] CHEN M, WANG C J, FANG W, et al. Electrospinning of calixarene functionalized polyacrylonitrile nanofiber membranes and application as an adsorbent and catalyst support[J]. Langmuir, 2013, 29 (38):126-127.
[14] 刁国旺, 张旺, 房伟,等. 一种杯芳烃聚丙烯腈复合纳米纤维的制备方法:102358962A[P].2012-02-22.DIAO Guowang, ZHANG Wang, FANG Wei, et al. A preparation method of calixarene polyacrylonitrile composite nanofibers: 102358962A [P].2012-02-22.
[15] LIN S, WEI W, WU X H, et al. Selective recovery of Pd(II) from extremely acidic solution using ion-imprinted chitosan fiber: adsorption performance and mechanisms [J]. Journal of Hazardous Materials, 2015, 299(6):10-17.
[16] 陶庭先, 吴之传, 孙志娟. 偕胺肟基纤维对Ni2+的吸附动力学[J]. 华南理工大学学报, 2003, 31(9):53-56.TAO Tingxian, WU Zhichuan, SUN Zhijuan. Kinetics of adsorption of nickel (Ⅱ) ion on fibre containing amidoxime groups [J]. Journal of South China University of Technology, 2003, 31(9):53-56.
[17] 李松林,周亚平,刘俊吉.物理化学:下册[M].5版.北京:高等教育出版社,2009:517,529.LI Songlin, ZHOU Yaping, LIU Junji. Physical Chemistry: Volume 2[M]. 5th ed. Beijing: Higer Education Press, 2009:517,529.
[18] LI X J, WANG X, WANG Q Q, et al. Effects of imidization temperature on the structure and properties of electrospun polyimide nanofibers [J]. Journal of Engineered Fibers and Fabrics, 2014, 9(4):33-38.
[19] 董世华, 胡运华. 冠醚聚合物的研究Ⅱ:以聚硫醚为主链的硫杂冠醚聚合物的合成及其络合性能[J]. 高分子学报, 1990, 1(4):399-405.DONG Shihua, HU Yunhua. Studies on polymeric crown ethers Ⅱ: syntheses and complexation properties of polymeric thiacrown ethers with polythiaether back-bone [J]. Acta Polymerica Sinica, 1990, 1(4):399-405.
[20] 李书干, 焦晓宁. 聚酰亚胺针刺织物与聚苯硫醚针刺物的热稳定性与燃烧性能对比[J].纺织学报,2012,33(12):35-39.LI Shugan, JIAO Xiaoning. Comparison of thermal stability and combustibility between PI and PPS needle punched fabrics [J]. Journal of Textile Research, 2012,33(12):35-39.
[21] 孔敏荣. 电荷半径比在无机化学中的应用[J]. 北京师范学院学报(自然科学版), 1992(1):65-68.KONG Minrong. Some application of charge-radius ratio in inorganic chemistry[J]. Journal of Beijing Teachers College (Natural Sciences Edition), 1992(1):65-68.
[22] 关勇, 孔繁荣. 电荷-半径比在无机化学中的某些应用[J]. 北京农学院学报, 1994(2):120-124.GUAN Yong, KONG Fanrong. Some applications of charge-radius ratio in inorganic chemistry[J]. Journal of Beijing Agricultural College, 1994(2):120-124.
[23] 凤权, 武丁胜, 桓珊,等. AOPAN/RC纳米纤维膜的制备及对金属离子吸附性能[J]. 高分子材料科学与工程, 2017, 33(8):140-144.FENG Quan, WU Dingsheng, HUAN Shan, et al. Preparation and metal ion adsorption properties of AOPAN/RC nanofibrous membrane[J].Polymer Materials Science and Engineering, 2017, 33(8):140-144.
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