均匀设计在微乳液法制备纳米氧化铝中的应用
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摘要
对多因素的复杂实验体系,均匀设计法能在不降低交互作用敏感性分析的前提下,可通过较少的实验次数获得可靠的数学模型,高效优化出最佳工艺条件。本文采用优化组合的U12+(6^6)均匀设计试验方案,考察了微乳液法制备纳米氧化铝前体的工艺条件,获得了氧化铝粉体的粒径与铝盐浓度、沉淀剂浓度、反应温度、表面活性剂与助表面活性剂的体积比、油相与表面活性剂的体积比5个关键因素之间的数学模型。利用该数学模型优化出的最佳制备工艺条件,制备出了氧化铝前体,该前体经1180℃焙烧,转晶为α-Al2O3粉体。α-Al2O3的一次粒子形状为棒状,一次粒子的Scherrer粒径为30nm左右,二次粒子的粒径D50为760nm。
For complex systems with multiple influence factors,reliable mathematical models could be obtained with few experiments by using the uniform-design method without decreasing interaction-sensitivity analysis,which can ben then used to derive the opitmal process conditions. A U12+(6^6) uniform-design test scheme was employed to investigate the optimum process conditions for preparing nano-alumina-precursor by microemulsion method. According to the experimental results, the mathematical model for relationship between the particle size of nano-alumina and the 5 factors of the concentration of aluminum salt, the precipitant concentration, the reaction temperature, the volume ratio of surfactant to cosurfactant, and the volume ratio of oil to surfactant, repsectively, was established. By using the mathematical model established, the optimum process conditions for preparing nano-alumina precursor were given. The α-Al2 O3 powder was then obtained by calcination at 1180℃ from the nano-alumina precursor preprared under the optimum process conditions. For the α-Al2 O3 powder, the primary particle shape was rod, the primary particle size was about 30 nm, and the secondary particle size(D50) was 760 nm.
For complex systems with multiple influence factors,reliable mathematical models could be obtained with few experiments by using the uniform-design method without decreasing interaction-sensitivity analysis,which can ben then used to derive the opitmal process conditions. A U12+(6^6) uniform-design test scheme was employed to investigate the optimum process conditions for preparing nano-alumina-precursor by microemulsion method. According to the experimental results, the mathematical model for relationship between the particle size of nano-alumina and the 5 factors of the concentration of aluminum salt, the precipitant concentration, the reaction temperature, the volume ratio of surfactant to cosurfactant, and the volume ratio of oil to surfactant, repsectively, was established. By using the mathematical model established, the optimum process conditions for preparing nano-alumina precursor were given. The α-Al2 O3 powder was then obtained by calcination at 1180℃ from the nano-alumina precursor preprared under the optimum process conditions. For the α-Al2 O3 powder, the primary particle shape was rod, the primary particle size was about 30 nm, and the secondary particle size(D50) was 760 nm.
引文
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[15]宋华,赵乐乐,宋华林,等.Al源种类对微乳液法制备固体超强酸催化剂异构化性能的影响[J].燃料化学学报,2015,43(10):1239-1244.SONG H,ZHAO L L,SONG H L,et al.Influence of aluminum species on the isomerization performance over solid superacid Pt-S2O82–/Zr O2-Al2O3[J].Journal of Fuel Chemistry and Technology,2015,43(10):1239-1244.
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[17]韩冰,李志宏.沉淀法制备纳米α-Al2O3的工艺[J].化学工业与工程,2006,23(6):512-515.HAN B,LI Z H.Technology of preparing alumina nanoparticles by precipitation method[J].Chemical Industry and Engineering,2006,23(6):512-515.
[18]曹娟,张永兴,汪效祖,等.硅烷偶联剂改性纳米氧化铝的条件探究[J].化工新型材料,2016,44(12):207-209.CAO J,ZHANG Y X,WANG X Z,et al.Study on the condition of silane coupling agent modifying Al2O3 nanoparticle[J].New Chemical Materials,2016,44(12):207-209.
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[2]王韵金,李宁宁,张永明,等.以乌海煤矸石为原料制备高纯氧化铝粉体[J].中国陶瓷,2014,50(5):55-59.WANG Y J,LI N N,ZHANG Y M,et al.Preparation of ultra-purity Al2O3 from wuhai coal gangue[J].China Ceramics,2014,50(5):55-59.
[3]SARKAR D,TIKKU S,THAPAR V,et al.Formation of zinc oxide nanoparticles of different shapes in water-in-oil microemulsion[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2011,381(1/3):123-129.
[4]朴玲钰,刘祥志,毛立娟,等.反相微乳液法制备纳米氧化铝[J].物理化学学报,2009,25(11):2232-2236.PIAO L Y,LIU X Z,MAO L J,et al.Preparation of nano-alumina by reverse microemulsion method[J].Acta Physico-Chimica Sinica,2009,25(11):2232-2236.
[5]WANG X H,LU G Z,GUO Y,et al.Preparation of high thermal-stabile alumina by reverse microemulsion method[J].Materials Chemistry&Physics,2005,90(s2/3):225-229.
[6]陈仕祥,刘红,王翠,等.微乳液法制备纳米Si O2/Ti O2及其光催化性能[J].化工进展,2012,31(5):1052-1056.CHEN S X,LIU H,WANG C,et al.Nanosized Si O2/Ti O2 particles prepared by microemulsion method and its photocatalytic activity[J].Chemical Industry and Engineering Progress,2012,31(5):1052-1056.
[7]宋华,汪淑影,李锋,等.微乳液法制备Pt/Al2O3催化剂及其催化氯代硝基苯选择加氢活性[J].化工进展,2011,30(4):771-776.SONG H,WANG S Y,LI F,et al.Preparation of Pt/Al2O3 catalyst by microemulsion and its activity in selective hydrogenation of chloronitrobenzene[J].Chemical Industry and Engineering Progress,2011,30(4):771-776.
[8]ZARUR A J,YING J Y.Reverse microemulsion synthesis of nanostructured complex oxides for catalytic combustion[J].Nature,2000,403:65-67.
[9]黄可龙,尹良果,刘素琴.反相微乳液法制备纳米Al2O3颗粒及其形成反应机理的研究[J].化学学报,2007,65(4):310-314.HUANG K L,YIN L G,LIU S Q.Study on preparation and formation mechanisms of Al2O3 nanoparticles by reverse micro emulsion[J].Journal of Chemical Industry and Engineering,2007,65(4):310-314.
[10]HOAR T P,SCHULMAN J H.Transparent water-in-oil dispersions:the oleopathic hydro-micelle[J].Nature,1943,152:102-103.
[11]方开泰.均匀设计与均匀设计表[M].北京:科学出版社,1994.FANG K T.Uniform design and uniform design table[M].Beijing:Science Press,1994.
[12]苏秀霞,支娟娟,李仲谨,等.均匀设计法优化β-环糊精微球的制备工艺[J].化工进展,2011,30(8):1785-1788.SU X X,ZHI J J,LI Z J,et al.Optimal preparation ofβ-cyclodextrin microsphere using uniform design[J].Chemical Industry and Engineering Progress,2011,30(8):1785-1788.
[13]苏秀霞,耿肖沙,李仲谨,等.均匀设计法优化一种高吸水性树脂的制备工艺[J].化工进展,2012,31(6):1269-1273.SU X X,GENG X S,LI Z J,et al.Optimal preparation of a type of super absorbent resin using uniform design[J].Chemical Industry and Engineering Progress,2012,31(6):1269-1273.
[14]夏之宁,谌其亭,穆小静,等.正交设计与均匀设计的初步比较[J].重庆大学学报(自然科学版),1999,22(5):112-117.XIA Z N,ZHAN Q T,MU X J,et al.Primary comparison of orthogonal and homogenous designs on experimental design and optimization[J].Journal of Chongqing University(Natural Science Edition),1999,22(5):112-117.
[15]宋华,赵乐乐,宋华林,等.Al源种类对微乳液法制备固体超强酸催化剂异构化性能的影响[J].燃料化学学报,2015,43(10):1239-1244.SONG H,ZHAO L L,SONG H L,et al.Influence of aluminum species on the isomerization performance over solid superacid Pt-S2O82–/Zr O2-Al2O3[J].Journal of Fuel Chemistry and Technology,2015,43(10):1239-1244.
[16]卢少元,贺蕴秋.表面活性剂在纳米氧化铝制备中的应用研究[J].材料导报,2006,20(s1):149-152.LU S Y,HE Y Q.Application of surfactant to synthesis of nanoalumina[J].Materials Review,2006,20(s1):149-152.
[17]韩冰,李志宏.沉淀法制备纳米α-Al2O3的工艺[J].化学工业与工程,2006,23(6):512-515.HAN B,LI Z H.Technology of preparing alumina nanoparticles by precipitation method[J].Chemical Industry and Engineering,2006,23(6):512-515.
[18]曹娟,张永兴,汪效祖,等.硅烷偶联剂改性纳米氧化铝的条件探究[J].化工新型材料,2016,44(12):207-209.CAO J,ZHANG Y X,WANG X Z,et al.Study on the condition of silane coupling agent modifying Al2O3 nanoparticle[J].New Chemical Materials,2016,44(12):207-209.
[19]黄仲涛,耿建铭.工业催化[M].北京:化学工业出版社,2008:62.HUANG Z T,GENG J M.Industrial catalysis[M].Beijing:Chemical Industry Press,2008:62.