低温等离子体改性碳纳米管及其对U(Ⅵ)的吸附性能研究
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摘要
采用低温等离子体法将O-磷酸乙醇胺(O-PEA)接枝到多壁碳纳米管表面(MWCNTs),并使用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、傅里叶变换红外光谱(FTIR)、X射线衍射(XRD)和拉曼光谱(Raman)表征改性前后的MWCNTs的物化性质.通过静态吸附实验研究改性碳纳米管对溶液中U(Ⅵ)的吸附容量,同时,还研究了吸附时间、pH、离子强度和温度对吸附性能的影响.结果表明,通过低温等离子体法改性后的MWCNTs(PTMWCNTs-4)对U(Ⅵ)的吸附性能最好,其吸附容量大约是未改性MWCNTs吸附量的3倍.改性后的MWCNTs吸附速率更快. PTMWCNTs-4对U(Ⅵ)的吸附在pH<7.0条件下不受离子强度影响,属于内层络合机理;而在pH>7.0条件下受离子强度影响,属于外层络合机理或离子交换.热力学数据表明,吸附过程放热且可自发进行.本文为U(Ⅵ)的有效去除提供了一种新型环保的改性方法.
Multiwalled carbon nanotubes(MWCNTs) grafted O-phosphoethanolamine(O-PEA) were prepared by nonthermal plasma technology for U(VI) adsorption. The modified MWCNTs were characterized by scanning electron microscopy(SEM), transmission electron microscopy(TEM), Fourier transform infrared spectrometer(FTIR), X-ray diffraction(XRD) and Raman spectra. The static adsorption study was carried out and the parameter effect on the adsorption capacity including contact time, pH, ionic strength and temperature were investigated. The results indicate that U(Ⅵ) adsorption on MWCNTs(PTMWCNTs-4) is the best, about three times that of the raw MWCNTs. The modified MWCNTs have a faster adsorption rate. The adsorption of U(Ⅵ) on PTMWCNTs-4 is dominated by the innersphere surface complexation at p H<7.0, whereas by the outer-sphere surface complexation or ion exchange at pH>7.0.Thermodynamic data show that the adsorption process is an exothermic and spontaneous process. This work provides a new environmental modification method for the efficient removal of U(Ⅵ).
Multiwalled carbon nanotubes(MWCNTs) grafted O-phosphoethanolamine(O-PEA) were prepared by nonthermal plasma technology for U(VI) adsorption. The modified MWCNTs were characterized by scanning electron microscopy(SEM), transmission electron microscopy(TEM), Fourier transform infrared spectrometer(FTIR), X-ray diffraction(XRD) and Raman spectra. The static adsorption study was carried out and the parameter effect on the adsorption capacity including contact time, pH, ionic strength and temperature were investigated. The results indicate that U(Ⅵ) adsorption on MWCNTs(PTMWCNTs-4) is the best, about three times that of the raw MWCNTs. The modified MWCNTs have a faster adsorption rate. The adsorption of U(Ⅵ) on PTMWCNTs-4 is dominated by the innersphere surface complexation at p H<7.0, whereas by the outer-sphere surface complexation or ion exchange at pH>7.0.Thermodynamic data show that the adsorption process is an exothermic and spontaneous process. This work provides a new environmental modification method for the efficient removal of U(Ⅵ).
引文
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21 Duan S,Liu X,Wang Y,Meng Y,Alsaedi A,Hayat T,Li J.Plasma Process Polym,2017,14:1600218
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24 Wang CX,Lv JC,Ren Y,Zhi T,Chen JY,Zhou QQ,Lu ZQ,Gao DW,Jin LM.Appl Surf Sci,2015,359:196-203
25 Shao D,Jiang Z,Wang X,Li J,Meng Y.J Phys Chem B,2009,113:860-864
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27 Song W,Liu M,Hu R,Tan X,Li J.Chem Eng J,2014,246:268-276
28 Das S,Pandey AK,Athawale AA,Manchanda VK.J Phys Chem B,2009,113:6328-6335
29 Chang K,Sun Y,Ye F,Li X,Sheng G,Zhao D,Linghu W,Li H,Liu J.Chem Eng J,2017,325:665-671
30 Chang K,Li X,Liao Q,Hu B,Hu J,Sheng G,Linghu W,Huang Y,Asiri AM,Alamry KA.Chem Eng J,2017,327:320-327
31 Sheng G,Li J,Shao D,Hu J,Chen C,Chen Y,Wang X.J Hazard Mater,2010,178:333-340
32 Shao D,Hu J,Wang X.Plasma Processes Polym,2010,7:977-985
33 Chong CT,Tan WH,Lee SL,Chong WWF,Lam SS,Valera-Medina A.Mater Chem Phys,2017,197:246-255
34 Zhang Z,Wang F,Yang W,Yang Z,Li A.Chem Eng J,2016,283:1522-1533
35 Duan S,Liu X,Wang Y,Shao D,Alharbi NS,Alsaedi A,Li J.J Taiwan Inst Chem Eng,2016,65:367-377
36 Wu FC,Tseng RL,Juang RS.Chem Eng J,2009,153:1-8
37 Hu B,Qiu M,Hu Q,Sun Y,Sheng G,Hu J,Ma J.ACS Sustain Chem Eng,2017,5:6924-6931
38 Zhang R,Chen C,Li J,Wang X.Appl Surf Sci,2015,349:129-137
39 Zong P,Gou J.J Mol Liq,2014,195:92-98
40 Zhao Y,Zong P,Li Y,Li K,Zhao X,Wang H,Liu S,Sun Y,He C.J Radioanal Nucl Chem,2015,305:361-369
41 Kütahyal?C,Eral M.J Nucl Mater,2010,396:251-256
42 Tian G,Geng J,Jin Y,Wang C,Li S,Chen Z,Wang H,Zhao Y,Li S.J Hazard Mater,2011,190:442-450
43 Li Z,Chen F,Yuan L,Liu Y,Zhao Y,Chai Z,Shi W.Chem Eng J,2012,210:539-546
44 Fang Q,Duan S,Zhang J,Li J,Leung KCF.J Mater Chem A,2017,5:2947-2958
45 Liu X,Chen H,Wang C,Qu R,Ji C,Sun C,Zhang Y.J Hazard Mater,2010,175:1014-1021
46 Kalavathy MH,Karthikeyan T,Rajgopal S,Miranda LR.J Colloid Interface Sci,2005,292:354-362
47 Zhang S,Zhang Y,Liu J,Xu Q,Xiao H,Wang X,Xu H,Zhou J.Chem Eng J,2013,226:30-38
48 Luo Z,Gao M,Yang S,Yang Q.Colloid Surface A,2015,482:222-230
49 Zhao Y,Li J,Zhang S,Chen H,Shao D.RSC Adv,2013,3:18952-18959
2 Liu X,Wang X,Li J,Wang X.Sci China Chem,2016,59:869-877
3 Yu S,Wang J,Song S,Sun K,Li J,Wang X,Chen Z,Wang X.Sci China Chem,2017,60:415-422
4 Pourcelot L,Masson O,Saey L,Conil S,Boulet B,Cariou N.J Environ Radioact,2017,171:74-82
5 Ganeev A,Gubal A,Korotetski B,Bogdanova O,Burakov B,Titova A,Solovyev N,Ivanenko N,Drobyshev E,Iakovleva E,Sillanp??M.Microchem J,2017,132:286-292
6 Min MZ,Luo XZ,Wang J,Jin YX,Wang RC.Sci China Ser D Earth Sci,2004,34:935-940(in Chinese)[闵茂中,罗兴章,王驹,金远新,王汝成.中国科学D辑:地球科学,2004,34:935-940]
7 Zhang Z,Duan S,Chen H,Zhang F,Hayat T,Alsaedi A,Li J.J Chem Eng Data,2018,63:1810-1820
8 Zhang S,Zeng M,Li J,Li J,Xu J,Wang X.J Mater Chem A,2014,2:4391-4397
9 Duan S,Xu X,Liu X,Wang Y,Hayat T,Alsaedi A,Meng Y,Li J.J Colloid Interface Sci,2018,513:92-103
10 Yao W,Wu Y,Pang H,Wang X,Yu S,Wang X.Sci China Chem,2018,61:812-823
11 Linghu W,Yang H,Sun Y,Sheng G,Huang Y.ACS Sustain Chem Eng,2017,5:5608-5616
12 Duan S,Li J,Liu X,Wang Y,Zeng S,Shao D,Hayat T.ACS Sustain Chem Eng,2016,4:3368-3378
13 Zhang S,Gao H,Li J,Huang Y,Alsaedi A,Hayat T,Xu X,Wang X.J Hazard Mater,2017,321:92-102
14 Liu X,Huang Y,Duan S,Wang Y,Li J,Chen Y,Hayat T,Wang X.Chem Eng J,2016,302:763-772
15 Lei Y,Zhao R,Zhan Y,Meng F,Zhong J,Yang X,Liu X.Chem Phys Lett,2010,496:139-142
16 Yoo KP,Kwon KH,Min NK,Lee MJ,Lee CJ.Sensor Actuator B-Chem,2009,143:333-340
17 He D,Peng Y,Yang H,Ma D,Wang Y,Chen K,Chen P,Shi J.Dyes Pigments,2013,99:395-401
18 Ballesteros B,de la Torre G,Ehli C,Aminur Rahman GM,Agulló-Rueda F,Guldi DM,Torres T.J Am Chem Soc,2007,129:5061-5068
19 Chen H,Li J,Shao D,Ren X,Wang X.Chem Eng J,2012,210:475-481
20 Yu XY,Luo T,Zhang YX,Jia Y,Zhu BJ,Fu XC,Liu JH,Huang XJ.ACS Appl Mater Interfaces,2011,3:2585-2593
21 Duan S,Liu X,Wang Y,Meng Y,Alsaedi A,Hayat T,Li J.Plasma Process Polym,2017,14:1600218
22 Garzia Trulli M,Sardella E,Palumbo F,Palazzo G,Giannossa LC,Mangone A,Comparelli R,Musso S,Favia P.J Colloid Interface Sci,2017,491:255-264
23 Duan S,Liu X,Wang Y,Shao D,Meng Y,Hayat T,Alsaedi A,Li J.RSC Adv,2017,7:21124-21127
24 Wang CX,Lv JC,Ren Y,Zhi T,Chen JY,Zhou QQ,Lu ZQ,Gao DW,Jin LM.Appl Surf Sci,2015,359:196-203
25 Shao D,Jiang Z,Wang X,Li J,Meng Y.J Phys Chem B,2009,113:860-864
26 Hongshan Z,Shengxia D,Lei C,Ahmed A,Tasawar H,Jiaxing L.Plasma Sci Technol,2017,19:115501
27 Song W,Liu M,Hu R,Tan X,Li J.Chem Eng J,2014,246:268-276
28 Das S,Pandey AK,Athawale AA,Manchanda VK.J Phys Chem B,2009,113:6328-6335
29 Chang K,Sun Y,Ye F,Li X,Sheng G,Zhao D,Linghu W,Li H,Liu J.Chem Eng J,2017,325:665-671
30 Chang K,Li X,Liao Q,Hu B,Hu J,Sheng G,Linghu W,Huang Y,Asiri AM,Alamry KA.Chem Eng J,2017,327:320-327
31 Sheng G,Li J,Shao D,Hu J,Chen C,Chen Y,Wang X.J Hazard Mater,2010,178:333-340
32 Shao D,Hu J,Wang X.Plasma Processes Polym,2010,7:977-985
33 Chong CT,Tan WH,Lee SL,Chong WWF,Lam SS,Valera-Medina A.Mater Chem Phys,2017,197:246-255
34 Zhang Z,Wang F,Yang W,Yang Z,Li A.Chem Eng J,2016,283:1522-1533
35 Duan S,Liu X,Wang Y,Shao D,Alharbi NS,Alsaedi A,Li J.J Taiwan Inst Chem Eng,2016,65:367-377
36 Wu FC,Tseng RL,Juang RS.Chem Eng J,2009,153:1-8
37 Hu B,Qiu M,Hu Q,Sun Y,Sheng G,Hu J,Ma J.ACS Sustain Chem Eng,2017,5:6924-6931
38 Zhang R,Chen C,Li J,Wang X.Appl Surf Sci,2015,349:129-137
39 Zong P,Gou J.J Mol Liq,2014,195:92-98
40 Zhao Y,Zong P,Li Y,Li K,Zhao X,Wang H,Liu S,Sun Y,He C.J Radioanal Nucl Chem,2015,305:361-369
41 Kütahyal?C,Eral M.J Nucl Mater,2010,396:251-256
42 Tian G,Geng J,Jin Y,Wang C,Li S,Chen Z,Wang H,Zhao Y,Li S.J Hazard Mater,2011,190:442-450
43 Li Z,Chen F,Yuan L,Liu Y,Zhao Y,Chai Z,Shi W.Chem Eng J,2012,210:539-546
44 Fang Q,Duan S,Zhang J,Li J,Leung KCF.J Mater Chem A,2017,5:2947-2958
45 Liu X,Chen H,Wang C,Qu R,Ji C,Sun C,Zhang Y.J Hazard Mater,2010,175:1014-1021
46 Kalavathy MH,Karthikeyan T,Rajgopal S,Miranda LR.J Colloid Interface Sci,2005,292:354-362
47 Zhang S,Zhang Y,Liu J,Xu Q,Xiao H,Wang X,Xu H,Zhou J.Chem Eng J,2013,226:30-38
48 Luo Z,Gao M,Yang S,Yang Q.Colloid Surface A,2015,482:222-230
49 Zhao Y,Li J,Zhang S,Chen H,Shao D.RSC Adv,2013,3:18952-18959