以CA为络合剂水热法合成硅酸锆粉体的研究
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摘要
以氧氯化锆(ZrOCl_2·8H_2O)和正硅酸乙酯(TEOS)为反应物,Li F作为矿化剂,柠檬酸(CA)作为络合剂,去离子水为溶剂,采用水热法在碱性条件下制备了形貌均匀的硅酸锆(ZrSiO_4)粉体。借助X射线衍射(XRD)、扫描电子显微镜(SEM)等测试手段,研究了CA/Zr比对络合能力的影响,以及制备过程中p H值、反应时间及反应温度等因素对ZrSiO_4粉体合成的影响。研究结果表明:当CA/Zr=0. 75时能够有效络合Zr~(4+)。通过调节p H值,可以获得片状、圆饼状等形貌的ZrSiO_4粉体。反应时间和反应温度,也会影响ZrSiO_4粉体的晶体生长过程,当水热反应温度为200℃,水热时间为24 h,p H值为9时制得的ZrSiO_4粉体形貌较均一。
ZrSiO_4 powders with uniform morphology were prepared by hydrothermal method under alkaline conditions,using zirconium oxychloride and tetraethoxysilane as raw materials,Li F as the mineralizer,citric acid( CA) as complexing agents,anddeionized water as solvent. The effects of CA/Zr molar ratio,p H value,reaction time and reaction temperature on synthesis of ZrSiO_4 powders were studied. The phase composition and microstructure of zircon powders were characterized by X-ray diffraction,scanning electronic microscopy. The results show that Zr~(4+) can be effectively complexed with a CA to Zr~(4+) mole ratio of 0. 75. ZrSiO_4 powder with different morphology such as flakes,doughnuts and rosettes can be obtained by adjusting the pH value. The hydrothermal time and temperature also affect the growth process of ZrSiO_4 crystal powder. The ZrSiO_4 powder with uniform morphology can be obtained by controlling hydrothermal temperature at 200 ℃ with 24 h when pH value is 9.
ZrSiO_4 powders with uniform morphology were prepared by hydrothermal method under alkaline conditions,using zirconium oxychloride and tetraethoxysilane as raw materials,Li F as the mineralizer,citric acid( CA) as complexing agents,anddeionized water as solvent. The effects of CA/Zr molar ratio,p H value,reaction time and reaction temperature on synthesis of ZrSiO_4 powders were studied. The phase composition and microstructure of zircon powders were characterized by X-ray diffraction,scanning electronic microscopy. The results show that Zr~(4+) can be effectively complexed with a CA to Zr~(4+) mole ratio of 0. 75. ZrSiO_4 powder with different morphology such as flakes,doughnuts and rosettes can be obtained by adjusting the pH value. The hydrothermal time and temperature also affect the growth process of ZrSiO_4 crystal powder. The ZrSiO_4 powder with uniform morphology can be obtained by controlling hydrothermal temperature at 200 ℃ with 24 h when pH value is 9.
引文
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[2]Pena P,De Aza S.The zircon thermal behavior:effect of impurities[J].Journal of the American Ceramic Society,1984,19(1):135-142.
[3]徐建华.硅酸锆基高温颜料的探讨[J].陶瓷研究,1994,9(3):139-143.
[4]陈静,曾令可,王慧,等.水溶液体系硅酸锆包裹硫硒化镉色料的研究[J].中国陶瓷工业,2017,24(5):1-8.
[5]朱振峰,朱敏.异晶包裹镉硒红颜料的研究进展及展望[J].陶瓷学报,2005,26(2):118-122.
[6]朱志斌.锆基色料的研究与发展[J].佛山陶瓷,2000(1):5-9.
[7]BondioliF,Ferrari A M,Leonelli C,et al.Syntheses of Fe2O3/Silicared inorganic inclusion pigments for ceramic applications[J].Materials Research Bulletin,1998,33(5):723-729.
[8]吕俊铎,吴秋芳.水解-共沉淀法制备硅酸锆包裹硫硒化镉色料[J].硅酸盐通报,2017,36(9):3197-3201.
[9]彭诚,张楚鑫,吕明,等.共沉淀法制备硅酸锆包裹炭黑及其高温稳定性[J].无机材料学报,2013,28(8):847-852.
[10]周杨帆,邓建成.溶胶共沉淀法合成硅酸锆包裹硫硒化镉大红颜料[J].湘潭大学自然科学学报,2011,33(1):69-72.
[11]宋晓岚,彭林,丁意,等.Zr SiO4/Cd(S1-xSex)包裹色料的水热合成[J].硅酸盐学报,2009,37(7):1264-1267.
[12]陆彩飞,王秀峰,苗鸿雁,等.纳米硅酸锆的水热合成[J].硅酸盐学报,2000,28(1):87-90.
[13]喻佑华,刘建磊,熊甜甜.溶胶-凝胶法低温合成硅酸锆粉体的研究[J].陶瓷学报,2018,28(3):382-385
[14]董雪亮,滕元成,曾冲盛,等.溶胶-凝胶法合成硅酸锆[J].中国粉体技术,2010,16(6):4-7.
[15]俞康泰,王永刚.溶胶凝胶法合成镨、钕硅酸锆色料的研究[J].陶瓷学报,2000,21(1):8-12.
[16]李小红,汪其堃.微乳液-水热法合成超细球形硅酸锆的研究[J].中国陶瓷,2018,54(10):17-20.
[17]Tartaj P.Zircon formation from nansized powders obtained by a reverse micelle process[J].Journal of the American Ceramic Society,2005,88(1):222-224.
[18]Song X L,Ding Y,Peng L,et al.Synthesis of Zr SiO4/Cd(S1-xSex)inclusion pigments by micro-emulsion method[J].Journal of the Chinese Ceramic Society,2010,38(5):974-978.
[19]严思明,廖咏梅,王柏云,等.新型络合剂的合成及其络合铁脱硫工艺研究[J].石油炼制与化工,2015,46(2):27-32.