超声时间对纳米结构化赤铁矿吸附Eu(Ⅲ)的影响及作用机制
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摘要
本文在空气气氛中热处理菱铁矿制备纳米结构化赤铁矿,研究了超声时间对制备的纳米结构化赤铁矿物化性质的影响,考察了反应时间、pH、离子强度、初始浓度对纳米结构化赤铁矿吸附Eu(Ⅲ)的影响.系列表征表明,热处理菱铁矿可形成纳米结构化赤铁矿,超声进一步降低了赤铁矿的粒径和结晶度,增大了比表面积.与纳米结构化赤铁矿相比,超声1 h得到的赤铁矿(PCH-3)具有最大的比表面积(29.37 m~2/g).批实验结果表明, T=288 K,pH 5.5时PCH-3对Eu(Ⅲ)的吸附具有最大的速率常数(K_2=3.49 g/(mg min))和容量(4.88 mg/g). X射线光电子能谱(XPS)分析证实,含氧官能团(特别是羟基)是纳米结构化赤铁矿富集Eu(Ⅲ)的主要吸附位点.而且适当的超声处理可显著提高纳米结构化赤铁矿表面反应性.该研究对矿物纳米结构化材料吸附重金属离子提供了重要的理论依据.
In this paper, the nanostructured hematite was prepared by heat treatment of siderite in air atmosphere. The influence of ultrasonic time on the physicochemical properties of nano structured hematite was studied. The effects of reaction time, pH, ionic strength and initial concentration on the adsorption of Eu(Ⅲ) hematite with different ultrasonic time were investigated. The series of characterization showed that nanostructured hematite can be formed by heating siderite. The size and crystallinity of nanoscale hematite were further reduced by ultrasound, resulting in increasement of the specific surface area. Compared with the nanostructured hematite without ultrasound, nanostructured hematite(PCH-3) after ultrasound for 1 h obtained the biggest specific surface area(29.37m~2/g). Batch experiments results indicated that PCH-3 had the maximum rate constant(K_2=3.49g/(mg min)) and the maximum adsorption capacity(4.88mg/g) for Eu(Ⅲ) adsorption at T=288K, pH 5.5. X-ray photoelectron spectroscopy(XPS) analysis confirmed that oxygen-containing functional groups(especially hydroxyl groups) were the main adsorption sites of Eu(Ⅲ) enriched by nano structured hematite. The results showed that proper ultrasound treatment can significantly improve the surface reactivity of the nano structured. This work is of great theoretical value for the adsorption of heavy metal ions by nanostructured mineral materials.
In this paper, the nanostructured hematite was prepared by heat treatment of siderite in air atmosphere. The influence of ultrasonic time on the physicochemical properties of nano structured hematite was studied. The effects of reaction time, pH, ionic strength and initial concentration on the adsorption of Eu(Ⅲ) hematite with different ultrasonic time were investigated. The series of characterization showed that nanostructured hematite can be formed by heating siderite. The size and crystallinity of nanoscale hematite were further reduced by ultrasound, resulting in increasement of the specific surface area. Compared with the nanostructured hematite without ultrasound, nanostructured hematite(PCH-3) after ultrasound for 1 h obtained the biggest specific surface area(29.37m~2/g). Batch experiments results indicated that PCH-3 had the maximum rate constant(K_2=3.49g/(mg min)) and the maximum adsorption capacity(4.88mg/g) for Eu(Ⅲ) adsorption at T=288K, pH 5.5. X-ray photoelectron spectroscopy(XPS) analysis confirmed that oxygen-containing functional groups(especially hydroxyl groups) were the main adsorption sites of Eu(Ⅲ) enriched by nano structured hematite. The results showed that proper ultrasound treatment can significantly improve the surface reactivity of the nano structured. This work is of great theoretical value for the adsorption of heavy metal ions by nanostructured mineral materials.
引文
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2 Linghu W,Yang H,Sun Y,Sheng G,Huang Y.ACS Sustain Chem Eng,2017,5:5608-5616
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19 Yang S,Zong P,Ren X,Wang Q,Wang X.ACS Appl Mater Interfaces,2012,4:6891-6900
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22 Li M,Liu H,Chen T,Lin W.Appl Geochem,2017,84:154-161
23 Liu H,Li M,Chen T,Chen C,Alharbi NS,Hayat T,Chen D,Zhang Q,Sun Y.Environ Sci Technol,2017,51:9227-9234
24 Sheng G,Dong H,Shen R,Li Y.Chem Eng J,2013,217:486-494
25 Sun Y,Zhang R,Ding C,Wang X,Cheng W,Chen C,Wang X.Geochim Cosmochim Acta,2016,180:51-65
26 Korichi S,Bensmaili A.J Hazard Mater,2009,169:780-793
27 Chmielarz L,Ku?trowski P,Dziembaj R,Cool P,Vansant EF.Catal Today,2007,119:181-186
28 Liu H,Chen T,Zou X,Qing C,Frost RL.J Raman Spectrosc,2013,44:1609-1614
29 Zoppi A,Lofrumento C,Castellucci EM,Sciau P.J Raman Spectrosc,2008,39:40-46
30 Zhang R,Liu H,Zou X,Qing C,Li M,Chen D.Environ Sci,2017,38:3519-3528
31 Duan S,Li J,Liu X,Wang Y,Zeng S,Shao D,Hayat T.ACS Sustain Chem Eng,2016,4:3368-3378
32 He Y,Chen Y G,Ye W M.Environ Earth Sci,2016,75:807-808
33 Yuan K,Taylor SD,Powell BA,Becker U.Surf Sci,2017,664:120-128
34 Naeimi S,Faghihian H.Sep Purif Technol,2017,175:255-265
35 Shao D,Hu J,Wang X.Plasma Processes Polym,2010,7:977-985
36 Hu J,Chen CL,Sheng GD,Li J,Chen Y,Wang X.Radiochim Acta,2010,98:421-429
37 Sun Y,Wu ZY,Wang X,Ding C,Cheng W,Yu SH,Wang X.Environ Sci Technol,2016,50:4459-4467
38 Aamrani SE,Giménez J,Rovira M,Seco F,GrivéM,Bruno J,Duro L,de Pablo J.Appl Surf Sci,2007,253:8794-8797
39 Li M,Liu H,Chen T,Hayat T,Alharbi NS,Chen C.J Mol Liquids,2017,236:445-451
40 Sharma P,Singh G,Tomar R.J Colloid Interface Sci,2009,332:298-308
41 Wu J,Li B,Liao J,Feng Y,Zhang D,Zhao J,Wen W,Yang Y,Liu N.J Environ Radioact,2009,100:914-920
42 Chen H,Huang S,Zhang Z,Liu Y,Wang X.Acta Chim Sinica,2017,75:560
43 Zhao G,Ren X,Gao X,Tan X,Li J,Chen C,Huang Y,Wang X.Dalton Trans,2011,40:10945-10952
44 Yang S,Wang X,Chen Z,Li Q,Niu B,Wang X.Prog Chem,2018,30:225-242(in Chinese)[杨姗也,王祥学,陈中山,李倩,韦犇犇,王祥科.化学进展.2018,30:225-242]
45 Liang Y,Gu P C,Wen Y,Yu S,Wang J,Wang X.Prog Chem,2017,29:1062-1071(in Chinese)[梁宇,顾鹏程,文姚,于淑君,王建,王祥科.化学进展,2017,29:1062-1071]
46 Tan X,Fang M,Li J,Lu Y,Wang X.J Hazard Mater,2009,168:458-465
47 Sheng G,Yang S,Sheng J,Hu J,Tan X,Wang X.Environ Sci Technol,2011,45:7718-7726
48 Sun Y,Wang Q,Chen C,Tan X,Wang X.Environ Sci Technol,2012,46:6020-6027
49 Song W,Liu M,Hu R,Tan X,Li J.Chem Eng J,2014,246:268-276
2 Linghu W,Yang H,Sun Y,Sheng G,Huang Y.ACS Sustain Chem Eng,2017,5:5608-5616
3 Liu J,Luo X,Wang J,Xiao T,Chen D,Sheng G,Yin M,Lippold H,Wang C,Chen Y.Environ Pollut,2017,224:445-453
4 Chen X,Zhang K,Yu H,Yu L,Ge H,Yue J.J Radioanal Nucl Ch,2018,7:1-9
5 Hu B,Hu Q,Chen C,Sun Y,Xu D,Sheng G.Chem Eng J,2017,322:66-72
6 Liu H,Zhu Y,Xu B,Li P,Sun Y,Chen T.J Hazard Mater,2017,322:488-498
7 Wang X,Sun Y,Alsaedi A,Hayat T,Wang X.Chem Eng J,2015,264:570-576
8 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
9 El Afifi EM,Attallah MF,Borai EH.J Environ Radioact,2016,151:156-165
10 Li M,Liu H,Zhu H,Gao H,Zhang S,Chen T.J Mol Liquids,2017,233:364-369
11 Borai EH,Harjula R,Malinen L,Paajanen A.J Hazard Mater,2009,172:416-422
12 Jang JH,Dempsey BA,Burgos WD.Water Res,2008,42:2269-2277
13 Minitha CR,Suresh R,Maity UK,Haldorai Y,Subramaniam V,Manoravi P,Joseph M,Rajendra Kumar RT.Ind Eng Chem Res,2018,57:1225-1232
14 Chen C,Hu J,Shao D,Li J,Wang X.J Hazard Mater,2009,164:923-928
15 Guo H,Stüben D,Berner Z.Appl Geochem,2007,22:1039-1051
16 Huber F,Schild D,Vitova T,Rothe J,Kirsch R,Sch?fer T.Geochim Cosmochim Acta,2012,96:154-173
17 Zhu Y,Liu H,Chen T,Xu B,Li P.J Mol Liquids,2016,218:565-570
18 Alexandratos VG,Behrends T,van Cappellen P.Environ Sci Technol,2017,51:2140-2150
19 Yang S,Zong P,Ren X,Wang Q,Wang X.ACS Appl Mater Interfaces,2012,4:6891-6900
20 Xing B,Chen T,Qing C,Liu H,Xie Q,Xie J.J Chin Ceram Soc,2016,44:1-6(in Chinese)[邢波波,陈天虎,庆承松,刘海波,谢巧勤,谢晶晶.硅酸盐学报,2016,44:1-6]
21 Li M,Sun Y,Liu H,Chen T,Hayat T,Alharbi NS,Chen C.ACS Sustain Chem Eng,2017,5:5493-5502
22 Li M,Liu H,Chen T,Lin W.Appl Geochem,2017,84:154-161
23 Liu H,Li M,Chen T,Chen C,Alharbi NS,Hayat T,Chen D,Zhang Q,Sun Y.Environ Sci Technol,2017,51:9227-9234
24 Sheng G,Dong H,Shen R,Li Y.Chem Eng J,2013,217:486-494
25 Sun Y,Zhang R,Ding C,Wang X,Cheng W,Chen C,Wang X.Geochim Cosmochim Acta,2016,180:51-65
26 Korichi S,Bensmaili A.J Hazard Mater,2009,169:780-793
27 Chmielarz L,Ku?trowski P,Dziembaj R,Cool P,Vansant EF.Catal Today,2007,119:181-186
28 Liu H,Chen T,Zou X,Qing C,Frost RL.J Raman Spectrosc,2013,44:1609-1614
29 Zoppi A,Lofrumento C,Castellucci EM,Sciau P.J Raman Spectrosc,2008,39:40-46
30 Zhang R,Liu H,Zou X,Qing C,Li M,Chen D.Environ Sci,2017,38:3519-3528
31 Duan S,Li J,Liu X,Wang Y,Zeng S,Shao D,Hayat T.ACS Sustain Chem Eng,2016,4:3368-3378
32 He Y,Chen Y G,Ye W M.Environ Earth Sci,2016,75:807-808
33 Yuan K,Taylor SD,Powell BA,Becker U.Surf Sci,2017,664:120-128
34 Naeimi S,Faghihian H.Sep Purif Technol,2017,175:255-265
35 Shao D,Hu J,Wang X.Plasma Processes Polym,2010,7:977-985
36 Hu J,Chen CL,Sheng GD,Li J,Chen Y,Wang X.Radiochim Acta,2010,98:421-429
37 Sun Y,Wu ZY,Wang X,Ding C,Cheng W,Yu SH,Wang X.Environ Sci Technol,2016,50:4459-4467
38 Aamrani SE,Giménez J,Rovira M,Seco F,GrivéM,Bruno J,Duro L,de Pablo J.Appl Surf Sci,2007,253:8794-8797
39 Li M,Liu H,Chen T,Hayat T,Alharbi NS,Chen C.J Mol Liquids,2017,236:445-451
40 Sharma P,Singh G,Tomar R.J Colloid Interface Sci,2009,332:298-308
41 Wu J,Li B,Liao J,Feng Y,Zhang D,Zhao J,Wen W,Yang Y,Liu N.J Environ Radioact,2009,100:914-920
42 Chen H,Huang S,Zhang Z,Liu Y,Wang X.Acta Chim Sinica,2017,75:560
43 Zhao G,Ren X,Gao X,Tan X,Li J,Chen C,Huang Y,Wang X.Dalton Trans,2011,40:10945-10952
44 Yang S,Wang X,Chen Z,Li Q,Niu B,Wang X.Prog Chem,2018,30:225-242(in Chinese)[杨姗也,王祥学,陈中山,李倩,韦犇犇,王祥科.化学进展.2018,30:225-242]
45 Liang Y,Gu P C,Wen Y,Yu S,Wang J,Wang X.Prog Chem,2017,29:1062-1071(in Chinese)[梁宇,顾鹏程,文姚,于淑君,王建,王祥科.化学进展,2017,29:1062-1071]
46 Tan X,Fang M,Li J,Lu Y,Wang X.J Hazard Mater,2009,168:458-465
47 Sheng G,Yang S,Sheng J,Hu J,Tan X,Wang X.Environ Sci Technol,2011,45:7718-7726
48 Sun Y,Wang Q,Chen C,Tan X,Wang X.Environ Sci Technol,2012,46:6020-6027
49 Song W,Liu M,Hu R,Tan X,Li J.Chem Eng J,2014,246:268-276
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