非化学计量对镁铝尖晶石的影响
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- 论文作者：范沐旭 ; 石干
- 年：2015
- 作者机构：中钢集团洛阳耐火材料研究院有限公司先进耐火材料国家重点实验室;
- 论文关键词：非化学计量 ; 镁铝尖晶石 ; 缺陷化学 ; 计量梯度 ; 烧结
- 会议召开时间：2015-10-25
- 会议录名称：2015耐火材料综合学术年会（第十三届全国不定形耐火材料学术会议和2015耐火原料学术交流会）论文集（4）
- 语种：中文
- 分类号：TQ175.1
- 学会代码：ZGJS
- 会议名称：2015耐火材料综合学术年会暨第十三届全国不定形耐火材料学术会议和2015耐火原料学术交流会
- 会议地点：中国山东青岛
- 主办单位：中国金属学会耐火材料分会、中国金属学会耐火材料分会不定形耐火材料技术委员会、耐火材料杂志社、中钢集团洛阳耐火材料研究院有限公司、武汉科技大学省部共建耐火材料与冶金国家重点实验室
- 学会名称：中国金属学会
- 页数：8
- 文件大小：2920k
- 原文格式：O
- 会议级别：全国
摘要
首先讨论了非化学计量镁铝尖晶石的缺陷化学,并阐述了非化学计量对镁铝尖晶石扩散、原位反应和烧结的影响。从非计量原位与预合成尖晶石两个方面入手,解释了目标组成与动态过程组成的区别;从晶粒表面Mg/MgO的蒸发和晶界处电荷补偿机制产生的计量梯度现象,分析了计量梯度对烧结及性能的影响。
引文
[1]Kim W,Saito F.Effect of grinding on synthesis of MgAl2 04 spinel from a powder mixture of Mg(OH)2 and Al(OH)3[J].Powder Technology,2000,113(1):109-113.
[2]Li J,Ikegami T,Lee J,et al.A wet-chemical process yielding reactive magnesium aluminate spinel(MgAl_2O_4)powderf J].Ceramics International,2001,27(4):481-489.
[3]Sarkar R,Chatterjee S,Mukherjee B,et al.Effect of alumina reactivity on the densification of reaction sintered nonstoichiometric spinel[J].Ceramics International,2003,29(2):195-198.
[4]Sarkar R,Banerjee G.Effect of compositional variation and fineness on the densification of MgO-Al_2O_3 compacts[J].Journal of the European Ceramic Society,1999,19(16):2893-2899.
[5]Sarkar R,Ghosh A,Das S K.Reaction sintered magnesia rich magnesium aluminate spinel:effect of alumina reactivity[J].Ceramics International,2003,29(4);407-411.
[6]Mora A,Gutierrez-Campos D,Lavelle C,et al.Evaluation of Bayer process gibbsite reactivity in magnesium aluminate spinel formation[J].Materials Science and Engineering:A,2007,454(16):139-143.
[7]Ganesh I,Bhattacharjee S.Saha B P,et al.A new sintering aid for magnesium aluminate spinel[J].Ceramics International,2001,27(1):773-779.
[8]Merac MRD,Reimanis IE,Smith C,et al.Effect of impurities and LiF additive in hot-pressed transparent magnesium aluminate spinel[J].International Journal of Applied Ceramic Technology,2013,10:E33-E48.
[9]Ganesh I,Teja K A.Thiyagarajan N,et al.Formation and densification behavior of magnesium aluminate spinel:The influence of CaO and moisture in the precursors[J].Journal of the American Ceramic Society,2005,88(10):2752-2761.
[10J Bhattaeharya G,Zhang S,Jayaseelan D,et al.Mineralizing effect of Li_2B_4O7 and Na_2B_4O7 on magnesium aluminate spinel formation[J].Journal of the American Ceramic Society,2007,90(1):97-106.
[11]Evstrop'ev K S,Smimov N A,Sharypin V V.Nanosize sintering additive based on B_2O_3 for obtaining ceramic from aluminum-magnesium spinel[J].Glass and Ceramics,2014,71(7-8):1573-8515.
[12]Rubat du M.The role of impurities,LIF,and processing on the sintering,microstructure,and optical properties of transparent polycrystalline magnesium aluminate(MgAl_2O_4)spinel[D].Colorado:Colorado School of Mines,2014.
[13]Matsui M,Takahashi T,Oda I.Influence of MgO vaporization on the final-stage sintering of MgO-Al_2O_3 spinel[J].Advances in ceramics,1984,10:562.
[14]Ting C,Lu H.Deterioration in the final-stage sintering of magnesium aluminate spinel[J].Journal of the American Ceramic Society,2000,83(7):1592-1598.
[15]Mazzoni A D.Sainz M A,Caballero A,et al.Formation and sintering of spinels(MgAl_2O_4)in reducing atmospheres[J].Materials Chemistry and Physics,2003,78(1):30-37.
[16]Hing P.Fabrication of translucent magnesium aluminate spinel and its compatibility in sodium vapour[J].Journal of Materials Science,1976,11(10):1919-1926.
[17]Ganesh I,01hero S M,Rebelo A H,et al.Formation and densification behavior of MgAl_2O_4 spinel:the influence of processing parameters[J].Journal of the American Ceramic Society,2008,91(6):1905-1911.
[18]Sarkar R,Das S K,Banerjee G.Calcination effect on magnesium hydroxide and aluminium hydroxide for the development of magnesium aluminate spinel[J].Ceramics International,2000,26(1):25-28.
[19]Ganesh I,Jaganatha Reddy G,Sundararajan G,et al.Influence of processing route on microstructure and mechanical properties of MgAl_2O_4 spinel[J].Ceramics International,2010,36(2):473-482.
[20]Mackenzie J D K,Temuujin J,Jadambaa T,et al.Mechanochemical synthesis and sintering behaviour of magnesium aluminate spinel[J].Journal of Materials Science,2000,35(22):5529-5535.
[21]Henkel L.Koch D,Grathwohl G.MgAl_2O_4-spinel synthesized by high-energy ball milling and reaction sintering[J].Journal of the American Ceramic Society,2009,92(4):805-811.
[22]Ghosh C,Ghosh A,Haldar M K.Studies on densification,mechanical,micro-structural and structure-properties relationship of magnesium abominate spinel refractory aggregates prepared from Indian magnesite[J].Materials Characterization,2014(11):84-91.
[23]Ganesh I.A review on magnesium aluminate(MgAl_2O_4)spinel:synthesis,processing and applications[J].International Materials Reviews,2013(2):63-112.
[24]Reimanis I,Kleebe H.A review On the sintering and microstracture development of transparent spinel(MgAl_2O_4)[J].Journal of the American Ceramic Society,2009,92(7):1472-1480.
[25]Goldstein A.Correlation between MgAl_2O_4-spinel structure,processing factors and functional properties of transparent parts(progress review)[J].Journal of the European Ceramic Society,2012,32(11):2869-2886.
[26]Murphy S T,Uberuaga B P,Ball J B,et al.Cation diffusion in magnesium aluminate spinel[J].Solid State Ionics,2009,180(1):1-8.
[27]Zhang P,DebRoy T,Seetharaman S.Interdiffusion in the MgOMgAl_2O_4spinel with or without some dopants[J].Metallurgical and Materials Transactions A,1996,27(8):2105-2114.
[28]Navias L.Preparation and properties of spinel made by vapor transport and diffusion in the system MgO-Al_2O_3[J].Journal of the American Ceramic society,1961,44(9):434-446.
[29]Reddy P R K,Cooper R A.Oxygen diffusion in magnesium aluminate spinel[J].Journal of the American Ceramic Society,1981,64(6):368-371.
[30]Rossir C,Fulrath R M.Epitaxial growth of spinel by reaction in the solid state[J].Journal of the American Ceramic Society,1963,46(3):145-149.
[31]Carter C B,Schmalzried H.The growth of spinel into Al_2O_3[J].Philosophical Magazine A,1985,52(2):207-224.
[32]Liu C,Chen J,Chen C.The growth of an epitaxial Mg-Al spinel layer on sapphire by solid-state reactions[J].Journal of Crystal Growth,2005,285:275-283.
[33]Carter C B,Rasmussen Y K.Growth of spinel particles on alumina thin films—I.Orientation relationships and shape of the particles[J].ActaMetallurgica et Materialia,1994,42(8):2729-2740.
[34]Carter C B,Rasmussen Y K.Growth of spinel particles on alumina thin films—II.Morphology and crystallography of the interface[J].ActaMetallurgica et Materialia,1994,42(8):2741-2752.
[35]Yasui I.Yamaguchi G,Kurosawa H.Interfacial phenomena and the orientation of spinel in MgO-Al_2O_3 solid state reaction[J].Journal of the Ceramic Association,1973,81:197.
[36]Hesse D,Bethge H.Solid state reactions for the epitaxial growth of spinel films[J].Journal of Crystal Growth,1983,65:69-76.
[37]Yalamac E,Carry C,Akkurt S.Microstructural development of interface layers between co-sintered alumina and spinel compacts[J].Journal of the European Ceramic Society,2011,31(9):1649-1659.
[38]Li D X,Pirouz P,Heuer A H,et al.A high-resolution electron microscopy study of MgO/Al_2O_3 interfaces and MgAl_2O_4 spinel formation[J].Philosophical Magazine A,1992,65(2):403-425.
[39]Proverbio E,Yasuoka M.Hirao TL,et al.Microstracture development during sintering in polycrystalline MgO?1.5Al_2O_3 spinel[J].Journal of the Ceramic Society of Japan,1993,101(3):256-262.
[40]Saalfeld V H,Jagodzinski H.Die entmischung Al_2O_3-tlbersMtigter Mg-Al-spinelle[J].Zeitschrift fur Kristallographie,1957,109(1-6):87-109.
[41]Bansal G K,Heuer A H.Precipitation in non-stoichiometric magnesium aluminate spinel[J].Philosophical Magazine,1974,29(4):709-722.
[42]Doukhan N,Doukhan J,Escaig B.Tem study of high temperature precipitation in(Al_2O_3)_n MgO spinels[J].Materials Research Bulletin,1976,11(2):125-133.
[43]Shirasuka K,Yamaguchi Goro,Momoda M.Differential thermal analysis of the nonstoichiometric spinel,MgO?nAl_2O_3(in Japanese)[J].Journal of the Ceramic Association,1976,84(10):523.
[44]Shuzo K,Zenbee N,Kenya H,et al.Effect of non-stoichiometry on microstracture and mechanical strength of Mg-Al spinel peramics(in Japanese)[J].Journal of the Ceramic Association,1979,87(5):230-237.
[45]Shuzo K,Kenya H.Zenbee N,et al.Precipitation strengthening in alumina-rich Mg-Al spinel ceramic(in Japanese)[J].Journal of the Ceramic Association,1976,88(7):411-417.
[46]Donlon W T,Mitchell T E.Heuer A H.Precipitation in non-stoichiometric spinel[J].Journal of Materials Science,1982,17(5):1389-1397.
[47]Panda P C,Raj R.Kinetics of Precipitation ofα-Al_2O_3 in polycrystalline supersaturated MgO·2Al_2O_3 spinel solid solution[J].Journal of the American Ceramic Society,1986,69(5):365-373.
[48]Ting C,Lu H.Defect reactions and the controlling mechanism in the sintering of magnesium aluminate spinel[J].Journal of the American Ceramic Society,1999,82(4):841-848.
[49]Sako E Y,Braulio M A L,Zinngrebe E,et al.Fundamentals and applications on in situ spinel formation mechanisms in Al_2O_3-MgO refractory castables[J].Ceramics International,2012,38(3):2243-2251.
[50]陈树江.相图分析及应用[M].北京:冶金工业出版社,2007:146.
[51]Duncan F C.Expansion during the formation of the magnesium aluminate spinel(MgAl_2O_4)from its basic oxide(MgO and Al_2O_3)powders[D].Alabama:The University of Alabama,2004.
[52]Wen Yan,Junfeng Chen,Nan li,et al.Preparation and characterization of porous MgO-Al_2O_3 refractory aggregates using an in-situ decomposition pore-forming technique[J].Ceramics International,2015,41(1):515-520.
[53]高振昕,平增福,张战营,等.耐火材料显微结构[M].北京:冶金工业出版社,2002:193.
[54]Kingery W D,Bowen H K,Uhlmann D R.陶瓷导论[M].清华大学新型陶艺与精细工艺国家重点实验室,译.北京:中国建筑工业出版社,1982:433-436.
[55]BROOK J R.Pore-grain boundary interactions and grain growth[J].Journal of the American Ceramic Society,1969,52(1);56-57.
[56]李代兵.刚玉-尖晶石质钢包透气砖抗热震性的研究[D].洛阳:洛阳耐火材料研究院,2008.
[57]Chiang Yet-Ming,David Kingery W.Grain-boundary migration in nonstoichiometric sohd solutions of magnesium aluminate spinel:I,grain growth studies[J].Journal of the American Ceramic Society,1989,72(2):271-277.
[58]Chiang Yet-Ming,David Kingery W.Grain-boundary migration in nonstoichiometric sohd solutions of magnesium aluminate spinel:II,effects of grain-boundary nonstoichiometry[J].Journal of the American Ceramic Society,1990,73(5):1153-1158.
[59]Nuns N,Beclin F,Crampon J.Grain-boundary characterization in a nonstoichiometric fine-grained magnesium aluminate spinel:Effects of defect segregation at the space-charge layers[J].Journal of the American Ceramic Society,2009,92(4):870-875.
[2]Li J,Ikegami T,Lee J,et al.A wet-chemical process yielding reactive magnesium aluminate spinel(MgAl_2O_4)powderf J].Ceramics International,2001,27(4):481-489.
[3]Sarkar R,Chatterjee S,Mukherjee B,et al.Effect of alumina reactivity on the densification of reaction sintered nonstoichiometric spinel[J].Ceramics International,2003,29(2):195-198.
[4]Sarkar R,Banerjee G.Effect of compositional variation and fineness on the densification of MgO-Al_2O_3 compacts[J].Journal of the European Ceramic Society,1999,19(16):2893-2899.
[5]Sarkar R,Ghosh A,Das S K.Reaction sintered magnesia rich magnesium aluminate spinel:effect of alumina reactivity[J].Ceramics International,2003,29(4);407-411.
[6]Mora A,Gutierrez-Campos D,Lavelle C,et al.Evaluation of Bayer process gibbsite reactivity in magnesium aluminate spinel formation[J].Materials Science and Engineering:A,2007,454(16):139-143.
[7]Ganesh I,Bhattacharjee S.Saha B P,et al.A new sintering aid for magnesium aluminate spinel[J].Ceramics International,2001,27(1):773-779.
[8]Merac MRD,Reimanis IE,Smith C,et al.Effect of impurities and LiF additive in hot-pressed transparent magnesium aluminate spinel[J].International Journal of Applied Ceramic Technology,2013,10:E33-E48.
[9]Ganesh I,Teja K A.Thiyagarajan N,et al.Formation and densification behavior of magnesium aluminate spinel:The influence of CaO and moisture in the precursors[J].Journal of the American Ceramic Society,2005,88(10):2752-2761.
[10J Bhattaeharya G,Zhang S,Jayaseelan D,et al.Mineralizing effect of Li_2B_4O7 and Na_2B_4O7 on magnesium aluminate spinel formation[J].Journal of the American Ceramic Society,2007,90(1):97-106.
[11]Evstrop'ev K S,Smimov N A,Sharypin V V.Nanosize sintering additive based on B_2O_3 for obtaining ceramic from aluminum-magnesium spinel[J].Glass and Ceramics,2014,71(7-8):1573-8515.
[12]Rubat du M.The role of impurities,LIF,and processing on the sintering,microstructure,and optical properties of transparent polycrystalline magnesium aluminate(MgAl_2O_4)spinel[D].Colorado:Colorado School of Mines,2014.
[13]Matsui M,Takahashi T,Oda I.Influence of MgO vaporization on the final-stage sintering of MgO-Al_2O_3 spinel[J].Advances in ceramics,1984,10:562.
[14]Ting C,Lu H.Deterioration in the final-stage sintering of magnesium aluminate spinel[J].Journal of the American Ceramic Society,2000,83(7):1592-1598.
[15]Mazzoni A D.Sainz M A,Caballero A,et al.Formation and sintering of spinels(MgAl_2O_4)in reducing atmospheres[J].Materials Chemistry and Physics,2003,78(1):30-37.
[16]Hing P.Fabrication of translucent magnesium aluminate spinel and its compatibility in sodium vapour[J].Journal of Materials Science,1976,11(10):1919-1926.
[17]Ganesh I,01hero S M,Rebelo A H,et al.Formation and densification behavior of MgAl_2O_4 spinel:the influence of processing parameters[J].Journal of the American Ceramic Society,2008,91(6):1905-1911.
[18]Sarkar R,Das S K,Banerjee G.Calcination effect on magnesium hydroxide and aluminium hydroxide for the development of magnesium aluminate spinel[J].Ceramics International,2000,26(1):25-28.
[19]Ganesh I,Jaganatha Reddy G,Sundararajan G,et al.Influence of processing route on microstructure and mechanical properties of MgAl_2O_4 spinel[J].Ceramics International,2010,36(2):473-482.
[20]Mackenzie J D K,Temuujin J,Jadambaa T,et al.Mechanochemical synthesis and sintering behaviour of magnesium aluminate spinel[J].Journal of Materials Science,2000,35(22):5529-5535.
[21]Henkel L.Koch D,Grathwohl G.MgAl_2O_4-spinel synthesized by high-energy ball milling and reaction sintering[J].Journal of the American Ceramic Society,2009,92(4):805-811.
[22]Ghosh C,Ghosh A,Haldar M K.Studies on densification,mechanical,micro-structural and structure-properties relationship of magnesium abominate spinel refractory aggregates prepared from Indian magnesite[J].Materials Characterization,2014(11):84-91.
[23]Ganesh I.A review on magnesium aluminate(MgAl_2O_4)spinel:synthesis,processing and applications[J].International Materials Reviews,2013(2):63-112.
[24]Reimanis I,Kleebe H.A review On the sintering and microstracture development of transparent spinel(MgAl_2O_4)[J].Journal of the American Ceramic Society,2009,92(7):1472-1480.
[25]Goldstein A.Correlation between MgAl_2O_4-spinel structure,processing factors and functional properties of transparent parts(progress review)[J].Journal of the European Ceramic Society,2012,32(11):2869-2886.
[26]Murphy S T,Uberuaga B P,Ball J B,et al.Cation diffusion in magnesium aluminate spinel[J].Solid State Ionics,2009,180(1):1-8.
[27]Zhang P,DebRoy T,Seetharaman S.Interdiffusion in the MgOMgAl_2O_4spinel with or without some dopants[J].Metallurgical and Materials Transactions A,1996,27(8):2105-2114.
[28]Navias L.Preparation and properties of spinel made by vapor transport and diffusion in the system MgO-Al_2O_3[J].Journal of the American Ceramic society,1961,44(9):434-446.
[29]Reddy P R K,Cooper R A.Oxygen diffusion in magnesium aluminate spinel[J].Journal of the American Ceramic Society,1981,64(6):368-371.
[30]Rossir C,Fulrath R M.Epitaxial growth of spinel by reaction in the solid state[J].Journal of the American Ceramic Society,1963,46(3):145-149.
[31]Carter C B,Schmalzried H.The growth of spinel into Al_2O_3[J].Philosophical Magazine A,1985,52(2):207-224.
[32]Liu C,Chen J,Chen C.The growth of an epitaxial Mg-Al spinel layer on sapphire by solid-state reactions[J].Journal of Crystal Growth,2005,285:275-283.
[33]Carter C B,Rasmussen Y K.Growth of spinel particles on alumina thin films—I.Orientation relationships and shape of the particles[J].ActaMetallurgica et Materialia,1994,42(8):2729-2740.
[34]Carter C B,Rasmussen Y K.Growth of spinel particles on alumina thin films—II.Morphology and crystallography of the interface[J].ActaMetallurgica et Materialia,1994,42(8):2741-2752.
[35]Yasui I.Yamaguchi G,Kurosawa H.Interfacial phenomena and the orientation of spinel in MgO-Al_2O_3 solid state reaction[J].Journal of the Ceramic Association,1973,81:197.
[36]Hesse D,Bethge H.Solid state reactions for the epitaxial growth of spinel films[J].Journal of Crystal Growth,1983,65:69-76.
[37]Yalamac E,Carry C,Akkurt S.Microstructural development of interface layers between co-sintered alumina and spinel compacts[J].Journal of the European Ceramic Society,2011,31(9):1649-1659.
[38]Li D X,Pirouz P,Heuer A H,et al.A high-resolution electron microscopy study of MgO/Al_2O_3 interfaces and MgAl_2O_4 spinel formation[J].Philosophical Magazine A,1992,65(2):403-425.
[39]Proverbio E,Yasuoka M.Hirao TL,et al.Microstracture development during sintering in polycrystalline MgO?1.5Al_2O_3 spinel[J].Journal of the Ceramic Society of Japan,1993,101(3):256-262.
[40]Saalfeld V H,Jagodzinski H.Die entmischung Al_2O_3-tlbersMtigter Mg-Al-spinelle[J].Zeitschrift fur Kristallographie,1957,109(1-6):87-109.
[41]Bansal G K,Heuer A H.Precipitation in non-stoichiometric magnesium aluminate spinel[J].Philosophical Magazine,1974,29(4):709-722.
[42]Doukhan N,Doukhan J,Escaig B.Tem study of high temperature precipitation in(Al_2O_3)_n MgO spinels[J].Materials Research Bulletin,1976,11(2):125-133.
[43]Shirasuka K,Yamaguchi Goro,Momoda M.Differential thermal analysis of the nonstoichiometric spinel,MgO?nAl_2O_3(in Japanese)[J].Journal of the Ceramic Association,1976,84(10):523.
[44]Shuzo K,Zenbee N,Kenya H,et al.Effect of non-stoichiometry on microstracture and mechanical strength of Mg-Al spinel peramics(in Japanese)[J].Journal of the Ceramic Association,1979,87(5):230-237.
[45]Shuzo K,Kenya H.Zenbee N,et al.Precipitation strengthening in alumina-rich Mg-Al spinel ceramic(in Japanese)[J].Journal of the Ceramic Association,1976,88(7):411-417.
[46]Donlon W T,Mitchell T E.Heuer A H.Precipitation in non-stoichiometric spinel[J].Journal of Materials Science,1982,17(5):1389-1397.
[47]Panda P C,Raj R.Kinetics of Precipitation ofα-Al_2O_3 in polycrystalline supersaturated MgO·2Al_2O_3 spinel solid solution[J].Journal of the American Ceramic Society,1986,69(5):365-373.
[48]Ting C,Lu H.Defect reactions and the controlling mechanism in the sintering of magnesium aluminate spinel[J].Journal of the American Ceramic Society,1999,82(4):841-848.
[49]Sako E Y,Braulio M A L,Zinngrebe E,et al.Fundamentals and applications on in situ spinel formation mechanisms in Al_2O_3-MgO refractory castables[J].Ceramics International,2012,38(3):2243-2251.
[50]陈树江.相图分析及应用[M].北京:冶金工业出版社,2007:146.
[51]Duncan F C.Expansion during the formation of the magnesium aluminate spinel(MgAl_2O_4)from its basic oxide(MgO and Al_2O_3)powders[D].Alabama:The University of Alabama,2004.
[52]Wen Yan,Junfeng Chen,Nan li,et al.Preparation and characterization of porous MgO-Al_2O_3 refractory aggregates using an in-situ decomposition pore-forming technique[J].Ceramics International,2015,41(1):515-520.
[53]高振昕,平增福,张战营,等.耐火材料显微结构[M].北京:冶金工业出版社,2002:193.
[54]Kingery W D,Bowen H K,Uhlmann D R.陶瓷导论[M].清华大学新型陶艺与精细工艺国家重点实验室,译.北京:中国建筑工业出版社,1982:433-436.
[55]BROOK J R.Pore-grain boundary interactions and grain growth[J].Journal of the American Ceramic Society,1969,52(1);56-57.
[56]李代兵.刚玉-尖晶石质钢包透气砖抗热震性的研究[D].洛阳:洛阳耐火材料研究院,2008.
[57]Chiang Yet-Ming,David Kingery W.Grain-boundary migration in nonstoichiometric sohd solutions of magnesium aluminate spinel:I,grain growth studies[J].Journal of the American Ceramic Society,1989,72(2):271-277.
[58]Chiang Yet-Ming,David Kingery W.Grain-boundary migration in nonstoichiometric sohd solutions of magnesium aluminate spinel:II,effects of grain-boundary nonstoichiometry[J].Journal of the American Ceramic Society,1990,73(5):1153-1158.
[59]Nuns N,Beclin F,Crampon J.Grain-boundary characterization in a nonstoichiometric fine-grained magnesium aluminate spinel:Effects of defect segregation at the space-charge layers[J].Journal of the American Ceramic Society,2009,92(4):870-875.