AlON透明陶瓷粉体的制备与改性工艺研究
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摘要
本文以纳米γ-Al2O3粉末和活性炭粉为原料,采用碳热还原法制备AlON粉体。首先研究了原料球磨时f间、原料配比、升温速度、烧结温度及保温时间等工艺对AlON粉体物相组成、粒度和比表面积的影响规律,然后研究了AlON粉体的球磨改性工艺对其比表面积及粒度分布的影响规律。
研究表明：球磨时间由12h增加到24h颗粒细化效果不明显；活性炭含量在5.4wt.%～5.8wt.%范围内时,均能获得单相AlON粉体；升温速度是影响合成粉末物相组成的关键因素之一,升温速度为10℃/min时,可得到的单相AlON,但以20℃/min升温时,合成产物中除主相AlON外还有残余Al2O3；提高烧结温度有利于碳热还原反应的进行,但是过高的温度会使粉料表层过度氮化成AlN:1750℃时,保温30min.60min和90min合成的粉末都为单相的AlON,而保温90min时粉饼表皮的粉末除了AlON相外还存在A1N相,即延长保温时间也有利于形成单相AlON,但是保温时间过长也会导致合成粉体表皮粉末中形成A1N。
AlON粉体球磨改性工艺研究表明：转速为250r/min时,延长球磨时间可起到细化AlON粉体颗粒及调整粒度分布的效果,球磨时间达36h时所获得的AlON粉体具有细粒度、窄分布的粒度分布特征。
In this paper AlON powder was prepared by carbothermal reduction method withγ-Al2O3 nano-powder and activated carbon powder as the raw material. First, the effect of ball-milling time of raw material, ratio of raw material, heating rate, sintering temperature and holding time on phase composition, particle size, specific surface area and micro-morphology of AlON powder were studed respectively. And the effect of milling technology of AlON powder on specific surface area and particle size distribution was also studied.
The results show that as time increases from 12h to 24h the degree of refinement of particle is weakening gradually. The composition of synthesized powder is single-phase AlON when the content of activated carbon powder ranges from 5.4wt.% to 5.6wt.%. Heating rate is one of the key points that have great influence on the phase composition of synthesized powder. It is single-phase AlON that can be prepared as the rate is 10℃/min, while mixed phase of Al2O3 and AlON can be prepared as the rate is 20℃/min. Increasing sintering temperature is beneficial to carbothermal reduction reaction. But when the temperature is too high, AlON powder on the surface will be reduced to AlN. Too long holding time will also result in formation of AlN. When holding 30min,60min and 90min at 1750℃, only synthesized powder for 90min has AlN at its surface.
According to the study on effect of milling technology of AlON powder we can know that the ball-milling speed and time have a great influence on specific surface area and particle size distribution at 250r/min. The powder for 36h is fine-grained and has a narrow distribution.
研究表明：球磨时间由12h增加到24h颗粒细化效果不明显；活性炭含量在5.4wt.%～5.8wt.%范围内时,均能获得单相AlON粉体；升温速度是影响合成粉末物相组成的关键因素之一,升温速度为10℃/min时,可得到的单相AlON,但以20℃/min升温时,合成产物中除主相AlON外还有残余Al2O3；提高烧结温度有利于碳热还原反应的进行,但是过高的温度会使粉料表层过度氮化成AlN:1750℃时,保温30min.60min和90min合成的粉末都为单相的AlON,而保温90min时粉饼表皮的粉末除了AlON相外还存在A1N相,即延长保温时间也有利于形成单相AlON,但是保温时间过长也会导致合成粉体表皮粉末中形成A1N。
AlON粉体球磨改性工艺研究表明：转速为250r/min时,延长球磨时间可起到细化AlON粉体颗粒及调整粒度分布的效果,球磨时间达36h时所获得的AlON粉体具有细粒度、窄分布的粒度分布特征。
In this paper AlON powder was prepared by carbothermal reduction method withγ-Al2O3 nano-powder and activated carbon powder as the raw material. First, the effect of ball-milling time of raw material, ratio of raw material, heating rate, sintering temperature and holding time on phase composition, particle size, specific surface area and micro-morphology of AlON powder were studed respectively. And the effect of milling technology of AlON powder on specific surface area and particle size distribution was also studied.
The results show that as time increases from 12h to 24h the degree of refinement of particle is weakening gradually. The composition of synthesized powder is single-phase AlON when the content of activated carbon powder ranges from 5.4wt.% to 5.6wt.%. Heating rate is one of the key points that have great influence on the phase composition of synthesized powder. It is single-phase AlON that can be prepared as the rate is 10℃/min, while mixed phase of Al2O3 and AlON can be prepared as the rate is 20℃/min. Increasing sintering temperature is beneficial to carbothermal reduction reaction. But when the temperature is too high, AlON powder on the surface will be reduced to AlN. Too long holding time will also result in formation of AlN. When holding 30min,60min and 90min at 1750℃, only synthesized powder for 90min has AlN at its surface.
According to the study on effect of milling technology of AlON powder we can know that the ball-milling speed and time have a great influence on specific surface area and particle size distribution at 250r/min. The powder for 36h is fine-grained and has a narrow distribution.
引文
[1]黄占杰.中红外导流罩及窗口材料的发展趋势.材料导报,1998,12(3)：30-33.
[2]李跃龙,黎建明,苏小平等.红外窗口和整流罩材料研究现状与发展趋势.人工晶体学报,2007,36(4)：877-884.
[3]王士维,袁贤阳,张芳等.AlON透明陶瓷的制备.中国空间科学学会空间材料专业委员会2009学术交流会,2009：59-62.
[4]姜华伟,杜洪兵,田庭燕,等.AlON透明陶瓷研究进展.硅酸盐通报,2009,28(2)：298-302.
[5]JosephMW, ThomasM H, Goldman LM. Recent advances in ALONTM optical ceramic. Proc. SPIE,2005,5786:71-82.
[6]Parimal J P, GaryA G, PeterG D. Transparent ceramics for armor and EM window applications. Proc. SPIE,2000,4120.
[7]Richard L G, Edward AM, Leonard E D. Transparentaluminum oxynitride and method of manufacture. United States, Patent,4720362,1988.
[8]施剑林,冯涛.无极光学透明材料——透明陶瓷,上海科学普及出版社,2008.
[9]COBLE R L. Transparent alumina and method of preparation. United States, Patent, 3026210,1962.
[10]王学荣,米晓云,卢歆.透明陶瓷的研究进展.硅酸盐学报,2007,35(12)：1671-1674.
[11]Hartnett T M. Optical properties of AlON. Infared Physics Technology, 1998,39:203-205.
[12]王介强.Y2O3,超微粉及其透明陶瓷的制备.东北大学学报,2003,18(6)：12-22.
[13]殷声.现代陶瓷及其应用.北京：科学技术出版社,1990.
[14]张晓娟,乔冠军,高宾.Al2O3透明陶瓷的显微组织和性能.中国陶瓷,2010,46(12)：21-24.
[15]杨秋红,徐军,宋平新等.Al2O3透明陶瓷显微结构的研究.功能材料与器件学报,2004,10(3)：299-302.
[16]靳玲玲,蒋志君,章健等.氧化钇透明陶瓷的研究进展.硅酸盐学报,2010,38(3)：521-526.
[17]王零森.特种陶瓷.中南大学出版社,1994.
[18]郝锋,彭鹏,刘艳改等.透明陶瓷的研究现状与发展展望.中国分金属矿工业导刊,2006,增刊(54)：164-166.
[19]齐建起,卢铁城,常相辉等MgAl2O4纳米透明陶瓷的制备及其透明机理.材料研究学报,2006,20(4)：367-371.
[20]马健,苗峰,吴娟等.YAG透明陶瓷的研究进展.西南民族大学学报·自然科学版,2007,33 (4)：836-840.
[21]张荣实.红外窗口/整流罩技术新进展.红外与激光工程,2007,36：114-119.
[22]周艳平,王岱峰,奚益明等.透明氮化铝陶瓷的制备.无机材料学报,1999,14(4)：674-678.
[23]MORSCHER G N, CHEN K C. Creep-resistance of development polycrystalline yttrium-aluminum garnet fibers. Ceram Eng Sci Proc,1994,14(7-8):181-188.
[24]李长青,张明福,左洪波等.影响透明陶瓷透光性能的困素.兵器材料科学与工程,2006,29(2)：26-30.
[25]应建新,张彬,崔鑫等.透明陶瓷透光性能的影响因素.强激光与粒子束,2011,23(3)：581-585.
[26]马健,苗峰,吴娟等.YAG透明陶瓷的研究进展,西南民族大学学报·自然科学版,2007,33(4)：836-840.
[27]Sullivan R M. A history view of ALONTM. Proc of SPIE,2005:23-32.
[28]田庭燕,杜洪兵,孙峰等.透明AlON陶瓷研究现状及应用.陶瓷,2008,12：20-23.
[29]庞微,伍登学,齐建起等.碳热还原法合成纯相氮氧化铝粉体的研究.稀有金属材料与工程,2007,36(1)：72-75.
[30]田庭燕,杜洪兵,孙峰等.AlON陶瓷透光性研究.陶瓷,2010,3：8-11.
[31]朱克武,张宁,才庆魁等.AlON陶瓷材料的研究进展.中国非金属矿工业导刊,66：16-19
[32]刘学建,袁贤阳,张芳等.碳热还原氮化工艺制备AlON透明陶瓷.无机材料学报,2010,25(7)：678-682.
[33]James W. M, Parimal P, Mingwei C et al. AlON:A brief history of its emergence and evolution. Journal of the European Ceramic Society 2009, (29):223-236.
[34]Wahl J M, Hartnett TM, Goldman L M, et al. Recent advances in AlONTM optical ceramic. Proceedings of SPIE,2005,2(19):3623-3632.
[35]张芳,王十维,张昭等.AlON粉体制备及透明陶瓷的烧结.稀有金属材料与工程,2009,38(2)：403-406.
[36]田庭燕,杜洪兵,姜华伟等.碳热还原法合成ALON粉体的研究.硅酸盐通报,2009,28(5)：1093-1096.
[37]魏巍.AlON透明陶瓷的制备与性能研究.武汉理工大学,2007.
[38]蔡杰,李文兰,张宝林等.自蔓延高温合成法在陶瓷领域的应用.真空电子技术,1996,2：39-42.
[39]田庭燕,杜洪兵,姜华伟等AlON透明陶瓷的制备与性能.硅酸盐学报,2010,38(8)： 1455-1458.
[40]郑捷, ForslundB1. ALON粉的稳定性和氧化行为.材料研究学报,1998,12(5)：497-506.
[2]李跃龙,黎建明,苏小平等.红外窗口和整流罩材料研究现状与发展趋势.人工晶体学报,2007,36(4)：877-884.
[3]王士维,袁贤阳,张芳等.AlON透明陶瓷的制备.中国空间科学学会空间材料专业委员会2009学术交流会,2009：59-62.
[4]姜华伟,杜洪兵,田庭燕,等.AlON透明陶瓷研究进展.硅酸盐通报,2009,28(2)：298-302.
[5]JosephMW, ThomasM H, Goldman LM. Recent advances in ALONTM optical ceramic. Proc. SPIE,2005,5786:71-82.
[6]Parimal J P, GaryA G, PeterG D. Transparent ceramics for armor and EM window applications. Proc. SPIE,2000,4120.
[7]Richard L G, Edward AM, Leonard E D. Transparentaluminum oxynitride and method of manufacture. United States, Patent,4720362,1988.
[8]施剑林,冯涛.无极光学透明材料——透明陶瓷,上海科学普及出版社,2008.
[9]COBLE R L. Transparent alumina and method of preparation. United States, Patent, 3026210,1962.
[10]王学荣,米晓云,卢歆.透明陶瓷的研究进展.硅酸盐学报,2007,35(12)：1671-1674.
[11]Hartnett T M. Optical properties of AlON. Infared Physics Technology, 1998,39:203-205.
[12]王介强.Y2O3,超微粉及其透明陶瓷的制备.东北大学学报,2003,18(6)：12-22.
[13]殷声.现代陶瓷及其应用.北京：科学技术出版社,1990.
[14]张晓娟,乔冠军,高宾.Al2O3透明陶瓷的显微组织和性能.中国陶瓷,2010,46(12)：21-24.
[15]杨秋红,徐军,宋平新等.Al2O3透明陶瓷显微结构的研究.功能材料与器件学报,2004,10(3)：299-302.
[16]靳玲玲,蒋志君,章健等.氧化钇透明陶瓷的研究进展.硅酸盐学报,2010,38(3)：521-526.
[17]王零森.特种陶瓷.中南大学出版社,1994.
[18]郝锋,彭鹏,刘艳改等.透明陶瓷的研究现状与发展展望.中国分金属矿工业导刊,2006,增刊(54)：164-166.
[19]齐建起,卢铁城,常相辉等MgAl2O4纳米透明陶瓷的制备及其透明机理.材料研究学报,2006,20(4)：367-371.
[20]马健,苗峰,吴娟等.YAG透明陶瓷的研究进展.西南民族大学学报·自然科学版,2007,33 (4)：836-840.
[21]张荣实.红外窗口/整流罩技术新进展.红外与激光工程,2007,36：114-119.
[22]周艳平,王岱峰,奚益明等.透明氮化铝陶瓷的制备.无机材料学报,1999,14(4)：674-678.
[23]MORSCHER G N, CHEN K C. Creep-resistance of development polycrystalline yttrium-aluminum garnet fibers. Ceram Eng Sci Proc,1994,14(7-8):181-188.
[24]李长青,张明福,左洪波等.影响透明陶瓷透光性能的困素.兵器材料科学与工程,2006,29(2)：26-30.
[25]应建新,张彬,崔鑫等.透明陶瓷透光性能的影响因素.强激光与粒子束,2011,23(3)：581-585.
[26]马健,苗峰,吴娟等.YAG透明陶瓷的研究进展,西南民族大学学报·自然科学版,2007,33(4)：836-840.
[27]Sullivan R M. A history view of ALONTM. Proc of SPIE,2005:23-32.
[28]田庭燕,杜洪兵,孙峰等.透明AlON陶瓷研究现状及应用.陶瓷,2008,12：20-23.
[29]庞微,伍登学,齐建起等.碳热还原法合成纯相氮氧化铝粉体的研究.稀有金属材料与工程,2007,36(1)：72-75.
[30]田庭燕,杜洪兵,孙峰等.AlON陶瓷透光性研究.陶瓷,2010,3：8-11.
[31]朱克武,张宁,才庆魁等.AlON陶瓷材料的研究进展.中国非金属矿工业导刊,66：16-19
[32]刘学建,袁贤阳,张芳等.碳热还原氮化工艺制备AlON透明陶瓷.无机材料学报,2010,25(7)：678-682.
[33]James W. M, Parimal P, Mingwei C et al. AlON:A brief history of its emergence and evolution. Journal of the European Ceramic Society 2009, (29):223-236.
[34]Wahl J M, Hartnett TM, Goldman L M, et al. Recent advances in AlONTM optical ceramic. Proceedings of SPIE,2005,2(19):3623-3632.
[35]张芳,王十维,张昭等.AlON粉体制备及透明陶瓷的烧结.稀有金属材料与工程,2009,38(2)：403-406.
[36]田庭燕,杜洪兵,姜华伟等.碳热还原法合成ALON粉体的研究.硅酸盐通报,2009,28(5)：1093-1096.
[37]魏巍.AlON透明陶瓷的制备与性能研究.武汉理工大学,2007.
[38]蔡杰,李文兰,张宝林等.自蔓延高温合成法在陶瓷领域的应用.真空电子技术,1996,2：39-42.
[39]田庭燕,杜洪兵,姜华伟等AlON透明陶瓷的制备与性能.硅酸盐学报,2010,38(8)： 1455-1458.
[40]郑捷, ForslundB1. ALON粉的稳定性和氧化行为.材料研究学报,1998,12(5)：497-506.