辐射接枝制备聚丙烯纤维基海水提铀吸附剂
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摘要
采用电子束预辐射接枝法将丙烯腈和丙烯酸接枝于聚丙烯(Polypropylene,PP)纤维上,并探讨了吸收剂量和反应温度对接枝率的影响。随后通过偕胺肟化反应制备出含偕胺肟基和羧基的PP纤维吸附剂。红外光谱数据表明,丙烯腈和丙烯酸成功接枝到PP纤维上,偕胺肟化反应将腈基转化为偕胺肟基,同时对改性前后PP纤维的表面形貌和热性能进行了表征。厦门海域真实海水吸附性能测试结果表明,所制备的PP纤维吸附剂铀吸附容量最高可达到0.81 mg·g~(-1)(吸附时间为68 d),PP纤维吸附剂的铀吸附容量与其接枝率和偕胺肟基密度不呈正相关。
Background: A recent estimate indicates that the land-based uranium sources are only able to last for about a century. Consequently, it is imperative to exploit new uranium resources with an economically feasible method. The uranium dissolved in seawater is about 4.5×109 t, much larger than the terrestrial sources, even though its concentration in seawater is low(about 3.3 μg·L-1). Hence, it is essential to develop techniques for mining uranium from seawater in order to satisfy the demand for uranium for nuclear power plants in the future. Purpose: The aim of this work is grafting of poly(amidoxime)(PAO) and poly(acrylic acid)(PAA) onto polypropylene(PP) fibers to prepare the PP-g-P(AO-co-AA) fibrous adsorbents for recovery of uranium from seawater. Methods: ThePP-g-P(AO-co-AA) fibrous adsorbents were synthesized by electron beam pre-irradiation induced graft polymerization of AN and AA, followed by amidoximation. The surface morphology, chemical structure and thermal performance of the pristine and modified PP fibers were analyzed by attenuated total reflection Fourier transform infrared(ATR-FTIR), scanning electron microscope(SEM) and thermogravimetric analysis(TGA), respectively. The adsorption capacities of uranium and other metal ions by PP-g-P(AO-co-AA) fibrous adsorbents were evaluated after 68 d of immersion in natural seawater. Results and Conclusion: The uranium adsorption capacity of PP-g-P(AO-co-AA) fibers reached 0.81 mg·g~(-1) after 68 d of contact with natural seawater, and the uranium adsorption capacity did not show positive correlation with the degree of grafting and AO density of PP-g-P(AO-co-AA) fibers.
Background: A recent estimate indicates that the land-based uranium sources are only able to last for about a century. Consequently, it is imperative to exploit new uranium resources with an economically feasible method. The uranium dissolved in seawater is about 4.5×109 t, much larger than the terrestrial sources, even though its concentration in seawater is low(about 3.3 μg·L-1). Hence, it is essential to develop techniques for mining uranium from seawater in order to satisfy the demand for uranium for nuclear power plants in the future. Purpose: The aim of this work is grafting of poly(amidoxime)(PAO) and poly(acrylic acid)(PAA) onto polypropylene(PP) fibers to prepare the PP-g-P(AO-co-AA) fibrous adsorbents for recovery of uranium from seawater. Methods: ThePP-g-P(AO-co-AA) fibrous adsorbents were synthesized by electron beam pre-irradiation induced graft polymerization of AN and AA, followed by amidoximation. The surface morphology, chemical structure and thermal performance of the pristine and modified PP fibers were analyzed by attenuated total reflection Fourier transform infrared(ATR-FTIR), scanning electron microscope(SEM) and thermogravimetric analysis(TGA), respectively. The adsorption capacities of uranium and other metal ions by PP-g-P(AO-co-AA) fibrous adsorbents were evaluated after 68 d of immersion in natural seawater. Results and Conclusion: The uranium adsorption capacity of PP-g-P(AO-co-AA) fibers reached 0.81 mg·g~(-1) after 68 d of contact with natural seawater, and the uranium adsorption capacity did not show positive correlation with the degree of grafting and AO density of PP-g-P(AO-co-AA) fibers.
引文
1 Pan H B,Kuo L J,Wai C M,et al.Elution of uranium and transition metals from amidoxime-based polymer adsorbents for sequestering uranium from seawater[J].Industrial&Engineering Chemistry Research,2016,55(15):4313-4320.DOI:10.1021/acs.iecr.5b03307.
2 Das S,Oyola Y,Mayes R T,et al.Extracting uranium from seawater:promising AF series adsorbents[J].Industrial&Engineering Chemistry Research,2016,55(15):4110-4117.DOI:10.1021/acs.iecr.5b03135.
3 Saito T,Brown S,Chatterjee S,et al.Uranium recovery from seawater:development of fiber adsorbents prepared via atom-transfer radical polymerization[J].Journal of Materials Chemistry A,2014,2(35):14674-14681.DOI:10.1039/C4TA03276D.
4 Schenk H J,Astheimer L,Witte E G,et al.Development of sorbers for the recovery of uranium from seawater-1.assessment of key parameters and screening studies of sorber materials[J].Separation Science and Technology,1982,17(11):1293-1308.DOI:10.1080/01496398208056103.
5 Kawai T,Saito K,Sugita K,et al.Comparison of amidoxime adsorbents prepared by cografting methacrylic acid and 2-hydroxyethyl methacrylate with acrylonitrile onto polyethylene[J].Industrial&Engineering Chemistry Research,2000,39(8):2910-2915.DOI:10.1021/ie990474a.
6 Piechowicz M,Abney C W,Zhou X,et al.Design,synthesis,and characterization of a bifunctional chelator with ultrahigh capacity for uranium uptake from seawater simulant[J].Industrial&Engineering Chemistry Research,2016,55(15):4170-4178.DOI:10.1021/acs.iecr.5b03304.
7饶林峰.辐射接枝技术的应用:日本海水提铀研究的进展及现状[J].同位素,2012,25(3):129-139.RAO Linfeng.Application of radiation grafting:progress and status of the extraction of uranium from seawater in Japan[J].Journal of Isotopes,2012,25(3):129-139.
8 Seko N,Katakai A,Hasegawa S,et al.Aquaculture of uranium in seawater by fabric-adsorbent submerged system[J].Nuclear Technology,2003,144(2):274-278.DOI:10.13182/NT03-2.
9 Kim J,Tsouris C,Mayes R T,et al.Recovery of uranium from seawater:a review of current status and future research needs[J].Separation Science and Technology,2013,48(3):367-387.DOI:10.1080/01496395.2012.712599.
10 Brown S,Yue Y F,Kuo L J,et al.Uranium adsorbent fibers prepared by atom-transfer radical polymerization(ATRP)from poly(vinyl chloride)-co-chlorinated poly(vinyl chloride)(PVC-co-CPVC)fiber[J].Industrial&Engineering Chemistry Research,2016,55(15):4139-4148.DOI:10.1021/acs.iecr.5b03355.
11熊洁,文君,胡胜,等.中国海水提铀研究进展[J].核化学与放射化学,2015,37(5):257-265.DOI:10.7538/HHX.2015.37.05.0257.XIONG Jie,WEN Jun,HU Sheng,et al.Progress in extracting uranium from seawater of China[J].Journal of Nuclear and Radiochemistry,2015,37(5):257-265.DOI:10.7538/HHX.2015.37.05.0257.
12 Xing Z,Hu J T,Wang M H,et al.Properties and evaluation of amidoxime-based UHMWPE fibrous adsorbent for extraction of uranium from seawater[J].Science China Chemistry,2013,56(11):1504-1509.DOI:10.1007/s11426-013-5002-x.
13 Hu J T,Ma H J,Xing Z,et al.Preparation of amidoximated ultrahigh molecular weight polyethylene fiber by radiation grafting and uranium adsorption test[J].Industrial&Engineering Chemistry Research,2016,55(15):4118-4124.DOI:10.1021/acs.iecr.5b03175.
14雷忠利,范友华.电子束预辐照聚丙烯接枝丙烯酸和丙烯腈的研究[J].辐射研究与辐射工艺学报,2005,25(3):151?154.LEI Zhongli,FAN Youhua.A study on grafting AA and AN onto PP fibers by EB preirradiation[J].Journal of Radiation Research and Radiation Processing,2005,25(3):151-154.
15 Choi S H,Nho Y C.Adsorption of UO22+by polyethylene adsorbents with amidoxime,carboxyl,and amidoxime/carboxyl group[J].Radiation Physics and Chemistry,2000,57(2):187-193.DOI:10.1016/S0969-806X(99)00348-5.
16 Kumar V,Bhardwaj Y K,Dubey K A,et al.Electron beam grafted polymer adsorbent for removal of heavy metal ion from aqueous solution[J].Separation Science and Technology,2006,41(14):3123-3139.DOI:10.1080/01496390600851673.
17 Oyola Y,Janke C J,Dai S.Synthesis,development,and testing of high-surface-area polymer-based adsorbents for the selective recovery of uranium from seawater[J].Industrial&Engineering Chemistry Research,2016,55(15):4149-4160.DOI:10.1021/acs.iecr.5b03981.
18缪小莉,李吉豪,向群,等.聚丙烯膜辐射接枝聚丙烯酰胺制备锂离子二次电池隔膜研究[J].核技术,2015,38(11):110302.DOI:10.11889/j.0253-3219.2015.hjs.38.110302.MIAO Xiaoli,LI Jihao,XIANG Qun,et al.Lithium-ion secondary battery separator prepared by radiation graft polymerization of polyacrylamide onto polypropylene membrane[J].Nuclear Techniques,2015,38(11):110302.DOI:10.11889/j.0253-3219.2015.hjs.38.110302.
19 Li R,Pang L J,Ma H J,et al.Optimization of molar content of amidoxime and acrylic acid in UHMWPEfibers for improvement of seawater uranium adsorption capacity[J].Journal of Radioanalytical and Nuclear Chemistry,2017,311:1771-1779.DOI:10.1007/s10967-016-5117-6.
20 Yue Y F,Mayes R T,Gill G,et al.Macroporous monoliths for trace metal extraction from seawater[J].RSC Advances,2015,5(62):50005-50010.DOI:10.1039/C5RA02131F.
21 Seko N,Katakai A,Tamada M,et al.Fine fibrous amidoxime adsorbent synthesized by grafting and uranium adsorption-elution cyclic test with seawater[J].Separation Science and Technology,2004,39(16):3753-3767.DOI:10.1081/SS-200042997.
2 Das S,Oyola Y,Mayes R T,et al.Extracting uranium from seawater:promising AF series adsorbents[J].Industrial&Engineering Chemistry Research,2016,55(15):4110-4117.DOI:10.1021/acs.iecr.5b03135.
3 Saito T,Brown S,Chatterjee S,et al.Uranium recovery from seawater:development of fiber adsorbents prepared via atom-transfer radical polymerization[J].Journal of Materials Chemistry A,2014,2(35):14674-14681.DOI:10.1039/C4TA03276D.
4 Schenk H J,Astheimer L,Witte E G,et al.Development of sorbers for the recovery of uranium from seawater-1.assessment of key parameters and screening studies of sorber materials[J].Separation Science and Technology,1982,17(11):1293-1308.DOI:10.1080/01496398208056103.
5 Kawai T,Saito K,Sugita K,et al.Comparison of amidoxime adsorbents prepared by cografting methacrylic acid and 2-hydroxyethyl methacrylate with acrylonitrile onto polyethylene[J].Industrial&Engineering Chemistry Research,2000,39(8):2910-2915.DOI:10.1021/ie990474a.
6 Piechowicz M,Abney C W,Zhou X,et al.Design,synthesis,and characterization of a bifunctional chelator with ultrahigh capacity for uranium uptake from seawater simulant[J].Industrial&Engineering Chemistry Research,2016,55(15):4170-4178.DOI:10.1021/acs.iecr.5b03304.
7饶林峰.辐射接枝技术的应用:日本海水提铀研究的进展及现状[J].同位素,2012,25(3):129-139.RAO Linfeng.Application of radiation grafting:progress and status of the extraction of uranium from seawater in Japan[J].Journal of Isotopes,2012,25(3):129-139.
8 Seko N,Katakai A,Hasegawa S,et al.Aquaculture of uranium in seawater by fabric-adsorbent submerged system[J].Nuclear Technology,2003,144(2):274-278.DOI:10.13182/NT03-2.
9 Kim J,Tsouris C,Mayes R T,et al.Recovery of uranium from seawater:a review of current status and future research needs[J].Separation Science and Technology,2013,48(3):367-387.DOI:10.1080/01496395.2012.712599.
10 Brown S,Yue Y F,Kuo L J,et al.Uranium adsorbent fibers prepared by atom-transfer radical polymerization(ATRP)from poly(vinyl chloride)-co-chlorinated poly(vinyl chloride)(PVC-co-CPVC)fiber[J].Industrial&Engineering Chemistry Research,2016,55(15):4139-4148.DOI:10.1021/acs.iecr.5b03355.
11熊洁,文君,胡胜,等.中国海水提铀研究进展[J].核化学与放射化学,2015,37(5):257-265.DOI:10.7538/HHX.2015.37.05.0257.XIONG Jie,WEN Jun,HU Sheng,et al.Progress in extracting uranium from seawater of China[J].Journal of Nuclear and Radiochemistry,2015,37(5):257-265.DOI:10.7538/HHX.2015.37.05.0257.
12 Xing Z,Hu J T,Wang M H,et al.Properties and evaluation of amidoxime-based UHMWPE fibrous adsorbent for extraction of uranium from seawater[J].Science China Chemistry,2013,56(11):1504-1509.DOI:10.1007/s11426-013-5002-x.
13 Hu J T,Ma H J,Xing Z,et al.Preparation of amidoximated ultrahigh molecular weight polyethylene fiber by radiation grafting and uranium adsorption test[J].Industrial&Engineering Chemistry Research,2016,55(15):4118-4124.DOI:10.1021/acs.iecr.5b03175.
14雷忠利,范友华.电子束预辐照聚丙烯接枝丙烯酸和丙烯腈的研究[J].辐射研究与辐射工艺学报,2005,25(3):151?154.LEI Zhongli,FAN Youhua.A study on grafting AA and AN onto PP fibers by EB preirradiation[J].Journal of Radiation Research and Radiation Processing,2005,25(3):151-154.
15 Choi S H,Nho Y C.Adsorption of UO22+by polyethylene adsorbents with amidoxime,carboxyl,and amidoxime/carboxyl group[J].Radiation Physics and Chemistry,2000,57(2):187-193.DOI:10.1016/S0969-806X(99)00348-5.
16 Kumar V,Bhardwaj Y K,Dubey K A,et al.Electron beam grafted polymer adsorbent for removal of heavy metal ion from aqueous solution[J].Separation Science and Technology,2006,41(14):3123-3139.DOI:10.1080/01496390600851673.
17 Oyola Y,Janke C J,Dai S.Synthesis,development,and testing of high-surface-area polymer-based adsorbents for the selective recovery of uranium from seawater[J].Industrial&Engineering Chemistry Research,2016,55(15):4149-4160.DOI:10.1021/acs.iecr.5b03981.
18缪小莉,李吉豪,向群,等.聚丙烯膜辐射接枝聚丙烯酰胺制备锂离子二次电池隔膜研究[J].核技术,2015,38(11):110302.DOI:10.11889/j.0253-3219.2015.hjs.38.110302.MIAO Xiaoli,LI Jihao,XIANG Qun,et al.Lithium-ion secondary battery separator prepared by radiation graft polymerization of polyacrylamide onto polypropylene membrane[J].Nuclear Techniques,2015,38(11):110302.DOI:10.11889/j.0253-3219.2015.hjs.38.110302.
19 Li R,Pang L J,Ma H J,et al.Optimization of molar content of amidoxime and acrylic acid in UHMWPEfibers for improvement of seawater uranium adsorption capacity[J].Journal of Radioanalytical and Nuclear Chemistry,2017,311:1771-1779.DOI:10.1007/s10967-016-5117-6.
20 Yue Y F,Mayes R T,Gill G,et al.Macroporous monoliths for trace metal extraction from seawater[J].RSC Advances,2015,5(62):50005-50010.DOI:10.1039/C5RA02131F.
21 Seko N,Katakai A,Tamada M,et al.Fine fibrous amidoxime adsorbent synthesized by grafting and uranium adsorption-elution cyclic test with seawater[J].Separation Science and Technology,2004,39(16):3753-3767.DOI:10.1081/SS-200042997.