羟基磷灰石微球的仿生合成及除氟性能
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摘要
以Ca(NO_3)_2·4H_2O和(NH_4)_3PO_4·3H_2O为反应物、β-环糊精/聚乙二醇(β-CD/PEG)复合物为模板,仿生合成羟基磷灰石(HA)微球。采用X-射线衍射分析、傅里叶变换红外吸收光谱、扫描电子显微镜等手段对产品的结构和形貌进行表征,结果表明当以0.4%～1.5%β-CD/PEG为模板时可合成直径为1～3μm的刺球状HA。通过正交试验L_(16)(4~5)得出HA除氟的最适宜操作工艺为:β-CD/PEG模板用量为0.8%、投加量为0.8 g·L~(-1)、氟离子浓度为8 ppm、振荡时间为12 h。在最适宜操作工艺下HA除氟效率可达99.70%,对氟离子的吸附容量为9.97 mg·g~(-1)。
Hydroxyapatite(HA)microspheres were biomimetic synthesized by using Ca(NO_3)_2·4 H_2O and(NH_4)_3PO_4·3 H_2O as raw materials and β-cyclodextrin/polyethylene glycol(β-CD/PEG)complex as templates.The structure and morphology of the samples were characterized by X-ray diffraction analysis,Fourier transform infrared absorption spectroscopy and scanning electron microscope.The results showed that HA burr-spheres with diameter of 1～3 μm could be synthesized with 0.4%～1.5%β-CD/PEG as templates.Orthogonal experiments L_(16)(4~5)indicated that the optimum parameters for defluorination efficiency of HA were as follows:the concentration of β-CD/PEG templates was 0.8%,the dosage of HA was 0.8 g·L~(-1),the concentration of fluorine ion was 8 ppm,the shaking time was 12 h.The defluorination efficiency of the obtained HA was 99.7%,and the fluoride adsorption capacity was 9.97 mg·g~(-1) at the optimum parameters.
Hydroxyapatite(HA)microspheres were biomimetic synthesized by using Ca(NO_3)_2·4 H_2O and(NH_4)_3PO_4·3 H_2O as raw materials and β-cyclodextrin/polyethylene glycol(β-CD/PEG)complex as templates.The structure and morphology of the samples were characterized by X-ray diffraction analysis,Fourier transform infrared absorption spectroscopy and scanning electron microscope.The results showed that HA burr-spheres with diameter of 1～3 μm could be synthesized with 0.4%～1.5%β-CD/PEG as templates.Orthogonal experiments L_(16)(4~5)indicated that the optimum parameters for defluorination efficiency of HA were as follows:the concentration of β-CD/PEG templates was 0.8%,the dosage of HA was 0.8 g·L~(-1),the concentration of fluorine ion was 8 ppm,the shaking time was 12 h.The defluorination efficiency of the obtained HA was 99.7%,and the fluoride adsorption capacity was 9.97 mg·g~(-1) at the optimum parameters.
引文
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[25]林皓,胡家朋,穆寄林,等.羟基磷灰石/活性炭复合吸附剂的制备及其除氟性能研究[J].人工晶体学报,2017,46(7): 1400-1407.
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[2]WHO(World Health Organization).Guideline for Drinking WaterQuality[R].First Addendum to third Edition,2006,1:375-377.
[3]Nunes-Pereira J,Lim R,Choudhary G,et al.Highly efficient removal of fluoride from aqueous media through polymer composite membranes[J].Separation and Purification Technology,2018,205:1-10.
[4]Belkada F D,Kitous O,Drouiche N,et al.Electrodialysis for fluoride and nitrate removal from synthesized photovoltaic industry wastewater[J].Separation and Purification Technology,2018,204:108-115.
[5]Huang H M,Liu J H,Zhang P,et al.Investigation on the simultaneous removal of fluoride,ammonia nitrogen and phosphate from semiconductor wastewater using chemical precipitation[J].Chemical Engineering Journal,2017,307:696-706.
[6]向文军,朱朝菊,魏世勇.几种赤铁矿的制备、表征及其对氟的吸附性能研究[J].化学研究与应用,2018,30(2): 290-296.
[7]Shivaprasad P,Singh P K,Saharan V K,et al.Synthesis of nano alumina for defluoridation of drinking water[J].Nano-Structures & Nano-Objects,2018,13: 109-120.
[8]朱庆霞,刘可春,李双,等.碳酸羟基磷灰石对水中氟离子的吸附研究[J].陶瓷学报,2017,38(6): 898-903.
[9]Talat M,Mohan S,Dixit V,et al.Effective removal of fluoride from water by coconut husk activated carbon in fixed bed column: Experimental and breakthrough curves analysis[J].Groundwater for Sustainable Development,2018,7: 48-55.
[10]Millar G J,Couperthwaite S J,Wellner D B,et al.Removal of fluoride ions from solution by chelating resin with imino-diacetate functionality[J].Journal of Water Process Engineering,2017,20: 113-122.
[11]Chen Z Z,Liu Y L,Mao L Z,et al.Effect of cation doping on the structure of hydroxyapatite and the mechanism of defluoridation[J].Ceramics International,2018,44(6): 6002-6009.
[12]Rajamohan N,Manivasagan R,Qasmi F A,et al.Defluoridation using hybrid clay-influence of process conditions and modeling[J].Desalin Water Treat,2017,97: 158-163.
[13]Chen Q,Cao L,Wang J L,et al.Improved cell adhesion and osteogenesis using a PLTGA (poly L-lactide,1,3-trimethylene carbonate,and glycolide) terpolymer by gelatin-assisted hydroxyapatite immobilization for bone regeneration[J].Journal of Materials Chemistry B,2018,6(2): 301-311.
[14]胡家朋,吴代赦,肖丽盈,等.羟基磷灰石的制备及其对水中氟离子的吸附[J].环境工程学报,2015,9(4): 1823-1830.
[15]Mehta D,Mondal P,Saharan V K,et al.Synthesis of hydroxyapatite nanorods for application in water defluoridation and optimization of process variables: Advantage of ultrasonication with precipitation method over conventional method[J].Ultrasonics Sonochemistry,2017,37: 56-70.
[16]He J Y,Zhang K S,Wu S B,et al.Performance of novel hydroxyapatite nanowires intreatment of fluoride contaminated water[J].Journal of Hazardous Materials,2016,303(16) :119-130.
[17]陈彰旭.咪唑-1-乙酸壳聚糖支架仿生合成羟基磷灰石[J].化工新型材料,2017,45(6): 230-235.
[18]邱超凡,肖秀峰,刘芳,等.β-环糊精为模板控制合成球状羟基磷灰石[J].人工晶体学报,2007,36(6): 1390-1394.
[19]郭明,费萌,马燕飞,等.环糊精自组装新型囊泡的合成及水溶性药物的包合性能研究[J].中国药学杂志,2015,50(6): 521-526.
[20]庄绪杰,李妍静,于东杰,等.β-环糊精/聚乙二醇复合物的制备及表征[J].化学世界,2014,9: 537-540.
[21]穆寄林,陈维俱,林皓,等.磁性羟基磷灰石的制备及其除氟性能研究[J].硅酸盐通报,2017,38(8):2659-2667.
[22]兰兴梅,王昌全,李冰,等.碳羟基磷灰石的合成对水中 Cd2+的去除特性研究[J].化学研究与应用,2018,30(4): 478-484.
[23]Poinern G E J,Ghosh M K,Ng Y J,et al.Defluoridation behavior of nanostructured hydroxyapatite synthesized through an ultrasonic and microwave combined technique[J].Journal of Hazardous Materials,2011,185(1): 29-37.
[24]万梦娇,王长秋,孟繁露,等.pH值对模拟体液中羟磷灰石晶体生长的调控[J].岩石矿物学杂志,2015,34(6): 950-956.
[25]林皓,胡家朋,穆寄林,等.羟基磷灰石/活性炭复合吸附剂的制备及其除氟性能研究[J].人工晶体学报,2017,46(7): 1400-1407.
[26]干成果,冯莉.负载羟基磷灰石活性炭的制备及除氟性能[J].功能材料,2013,44(22): 3243-3246.
[27]李玲,朱志良,仇雁翎,等.缺钙型羟基磷灰石对溶液中氟离子的吸附作用研究[J].环境科学,2010,31(6): 1554-1559.
[28]Jiménez-Reyes M,Solache-Ríoso M.Sorption behavior of fluoride ions from aqueous solutions by hydroxyapatite[J].Journal of Hazardous Materials,2010,180(1-3): 297-302.