Mg-α-SiAlON/MgO复合材料中Mg-α-SiAlON的原位合成
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摘要
为改善低品位Mg基材料高温性能,采用烧结Mg砂、金属Al粉、单质Si粉和Al_2O_3粉为主要原料,制备了Mg-α-SiAlON/MgO复合材料。通过XRD、SEM及EDS等检测手段,研究了不同原料质量分数及氮化温度条件下Mg-α-SiAlON/MgO复合材料中Mg-α-SiAlON的原位合成,结合热力学分析确定了合成Mg-α-SiAlON的气氛条件并分析了合成Mg-α-SiAlON的反应机制。结果表明:1 550℃时的氮、氧分压满足合成Mg-α-SiAlON的热力学条件。当烧结Mg砂粉、Al粉、Si粉和Al_2O_3粉的质量分数之和为40wt%时,1 550℃保温3h氮化后的Mg-α-SiAlON/MgO复合材料中板片状Mg-α-SiAlON相生成量最高可达32.1%,且相互交错构成骨架,将低熔点物相包裹其中。利用烧结Mg砂原位氮化制备Mg-α-SiAlON/MgO复合材料,有利于提高Mg基材料的抗热震性能。
In order to improve the high temperature properties of low grade magnesium-based material,Mg-α-SiAlON/MgO composites were prepared using sintered magnesia,Al metal powder,Si powder and Al_2O_3 powder as the raw material,the Mg-α-SiAlON phase in-situ forming in the Mg-α-SiAlON/MgO composites sintered at different temperature and mass fraction were determined by XRD,SEM and EDS.The synthesis atmosphere conditions of Mg-α-SiAlON were determined by thermodynamic analysis and the reaction mechanism of Mg-α-SiAlON phase were explained.The experiment results show that the partial pressure of nitrogen and oxygen at 1 550℃ satisfies the thermodynamic requirement for the synthesis of Mg-α-SiAlON.When the total mass fraction of sintered magnesia powder,Al metal powder,Si powder and Al_2O_3 powder is 40 wt%,the content of Mg-α-SiAlON phase with plate-like shape is as high as 32.1%in Mg-α-SiAlON/MgO composites nitrided at 1 550℃for 3 h.Mg-α-SiAlON phase interlace to form a skeleton and envelope the low melting phase inside of it.The in-situ synthesis of Mg-α-SiAlON/MgO composites from sintered magnesia by nitridation is beneficial for improving the thermal shock resistance of magnesium-based material.
In order to improve the high temperature properties of low grade magnesium-based material,Mg-α-SiAlON/MgO composites were prepared using sintered magnesia,Al metal powder,Si powder and Al_2O_3 powder as the raw material,the Mg-α-SiAlON phase in-situ forming in the Mg-α-SiAlON/MgO composites sintered at different temperature and mass fraction were determined by XRD,SEM and EDS.The synthesis atmosphere conditions of Mg-α-SiAlON were determined by thermodynamic analysis and the reaction mechanism of Mg-α-SiAlON phase were explained.The experiment results show that the partial pressure of nitrogen and oxygen at 1 550℃ satisfies the thermodynamic requirement for the synthesis of Mg-α-SiAlON.When the total mass fraction of sintered magnesia powder,Al metal powder,Si powder and Al_2O_3 powder is 40 wt%,the content of Mg-α-SiAlON phase with plate-like shape is as high as 32.1%in Mg-α-SiAlON/MgO composites nitrided at 1 550℃for 3 h.Mg-α-SiAlON phase interlace to form a skeleton and envelope the low melting phase inside of it.The in-situ synthesis of Mg-α-SiAlON/MgO composites from sintered magnesia by nitridation is beneficial for improving the thermal shock resistance of magnesium-based material.
引文
[1]徐殿利.“十三五”期间耐火材料行业发展相关问题的思考[J].耐火材料,2016,50(2):81-84.XU D L.Thoughts for development of China’s refractories industry during“the 13th Five-Year-Plan”period[J].Refractories,2016,50(2):81-84(in Chinese).
[2]闫平科,卢智强,赵永帅,等.低品位菱镁矿加压碳酸化法提纯试验研究[J].硅酸盐通报,2015,34(11):3372-3376.YAN P K,LU Z Q,ZHAO Y S,et al.Purification of pressural carbonation for a low-grade magnesite[J].Bulletin of the Chinese Ceramic Society,2015,34(11):3372-3376(in Chinese).
[3]LI X C,CHEN S S,DING H,et al.Preparation and characterization of corundum-mullite-spinel refractories from lowgrade bauxite and magnesite ores[J].Journal of the Ceramic Society of Japan,2016,124(1):88-91.
[4]任瑞辰,王志恒,李彩霞,等.辽宁海城某低品位菱镁矿选矿试验研究[J].非金属矿,2017,40(4):67-69.REN R C,WANG Z H,LI C X,et al.Research on low grade magnesite processing from Liaoning Haicheng[J].Non-Metallic Mines,2017,40(4):67-69(in Chinese).
[5]罗旭东,曲殿利,张国栋.氧化镧对菱镁矿风化石制备镁铝尖晶石组成结构的影响[J].稀土,2012,33(4):59-63.LUO X D,QU D L,ZHANG G D.Influence of lanthanum on composition and structure of Mg-Al spinel material prepared from decomposed magnesite[J].Chinese Rare Earths,2012,33(4):59-63(in Chinese).
[6]罗旭东,曲殿利,张国栋,等.氧化铬对镁橄榄石材料结构及性能的影响[J].材料热处理学报,2013,34(1):21-25.LUO X D,QU D L,ZHANG G D,et al.Effect of Cr2O3addition on structure and properties of forsterite synthesized from low-grade magnesite and natural silica[J].Transactions of Materials and Heat Treatment,2013,34(1):21-25(in Chinese).
[7]罗旭东,曲殿利,张国栋.Eu3+、Dy3+和Er3+对制备堇青石晶相转变的对比表征[J].复合材料学报,2013,30(4):148-155.LUO X D,QU D L,ZHANG G D.Characterization comparison of Eu3+,Dy3+and Er3+on phase transition of cordierite[J].Acta Materiae Compositae Sinica,2013,30(4):148-155(in Chinese).
[8]LI Y W,WANG P L,CHEN W W,et al.Formation behavior,microstructure and mechanical properties of multi-cation alpha sialons containing calcium and neodyium[J].Journal of the European Ceramic Society,2001,21(9):1273-1279.
[9]AVCIOGLU S,KURAMA S.Investigation of the influence of initial powder size on the optical properties of Dy-α-SiAlONceramics fabricated by gas pressure sintering[J].Ceramics International,2017,43(s1):449-454.
[10]KHAN R M A,MALKI M M A,HAKEEM A S,et al.Development of a single-phase Ca-α-SiAlON ceramic from nano-sized precursors using spark plasma sintering[J].Materials Science&Engineering A,2016,673:243-249.
[11]YI X M,NIU J,TOMOHIRO A,et al.Spark plasma sintering behavior of combustion synthesized(Y,Ca)-α-SiAlON[J].Ceramics International,2016,42(14):15687-15693.
[12]YANG Z F,WANG H,MIN X M,et al.Translucent Li-α-SiAlON ceramics prepared by spark plasma sintering rapid communications of the American ceramic society[J].Journal of the American Ceramic Society,2010,93(11):3549-3551.
[13]孙洋,陈树江,田琳,等.MgO-sialon/MgO复合材料中Mgsialon片晶的形成和表征[J].复合材料学报,2017,34(3):604-610.SUN Y,CHEN S J,TIAN L,et al.Formation and characterization of Mg-sialon platelet grain in Mg-sialon/MgO composites[J].Acta Materiae Compositae Sinica,2017,34(3):604-610(in Chinese).
[14]YE F,LIU C F,LIU L M.Microstructure and mechanical properties of multi-cation containingα-sialons[J].Ceramics International,2009,35(2):725-731.
[15]刘新,曲殿利,郭玉香,等.自扩散式高温氮化制备Mg-α/β-sialon复相陶瓷[J].人工晶体学报,2016,45(2):435-440.LIU X,QU D L,GUO Y X,et al.Synthesis of Mg-α/β-sialon composites by high temperature self-diffusion nitridation reaction[J].Journal of Synthetic Crystals,2016,45(2):435-440(in Chinese).
[16]桑绍柏,李亚伟,杨纯艳,等.原位反应制备Mg-α-Sialon结合镁质耐火材料研究[J].武汉科技大学学报(自然科学版),2005,28(4):338-342.SANG S B,LI Y W,YANG C Y,et al.Mg-α-Sialon bonded magnesia refractories prepared by in-situ nitridetion process[J].Journal of Wuhan University of Science and Technology(Natural Science Edition),2005,28(4):338-342(in Chinese).
[17]李红霞.耐火原料手册[M].北京:冶金工业出版,2007.LI H X.Manual of refractory materials[M].Beijing:Metallurgical Industry Press,2007(in Chinese).
[18]WANG P L,LI Y W,YAN D S.Effect of amount and atomic ratio of dual modifiers Ca and Mg on phase formation and mechanical properties of Ca,Mg-α-sialons[J].Journal of Materials Science,2000,35(7):1585-1588.
[19]LI Y W,SANG S B,JIN S L,et al.Synthesis of Mg-α-sialon from the mixture of silicon,aluminum and magnesia powders in a flowing nitrogen atmosphere[J].Journal of Materials Science,2006,41(18):5815-5819.
[20]WANG P L,ZHANG C,SUN W Y,et al.Characteristics of Ca-α-sialon phase formation,microstructure and mechanical properties[J].Journal of European Ceramic Society,1999,19(5):553-560.
[2]闫平科,卢智强,赵永帅,等.低品位菱镁矿加压碳酸化法提纯试验研究[J].硅酸盐通报,2015,34(11):3372-3376.YAN P K,LU Z Q,ZHAO Y S,et al.Purification of pressural carbonation for a low-grade magnesite[J].Bulletin of the Chinese Ceramic Society,2015,34(11):3372-3376(in Chinese).
[3]LI X C,CHEN S S,DING H,et al.Preparation and characterization of corundum-mullite-spinel refractories from lowgrade bauxite and magnesite ores[J].Journal of the Ceramic Society of Japan,2016,124(1):88-91.
[4]任瑞辰,王志恒,李彩霞,等.辽宁海城某低品位菱镁矿选矿试验研究[J].非金属矿,2017,40(4):67-69.REN R C,WANG Z H,LI C X,et al.Research on low grade magnesite processing from Liaoning Haicheng[J].Non-Metallic Mines,2017,40(4):67-69(in Chinese).
[5]罗旭东,曲殿利,张国栋.氧化镧对菱镁矿风化石制备镁铝尖晶石组成结构的影响[J].稀土,2012,33(4):59-63.LUO X D,QU D L,ZHANG G D.Influence of lanthanum on composition and structure of Mg-Al spinel material prepared from decomposed magnesite[J].Chinese Rare Earths,2012,33(4):59-63(in Chinese).
[6]罗旭东,曲殿利,张国栋,等.氧化铬对镁橄榄石材料结构及性能的影响[J].材料热处理学报,2013,34(1):21-25.LUO X D,QU D L,ZHANG G D,et al.Effect of Cr2O3addition on structure and properties of forsterite synthesized from low-grade magnesite and natural silica[J].Transactions of Materials and Heat Treatment,2013,34(1):21-25(in Chinese).
[7]罗旭东,曲殿利,张国栋.Eu3+、Dy3+和Er3+对制备堇青石晶相转变的对比表征[J].复合材料学报,2013,30(4):148-155.LUO X D,QU D L,ZHANG G D.Characterization comparison of Eu3+,Dy3+and Er3+on phase transition of cordierite[J].Acta Materiae Compositae Sinica,2013,30(4):148-155(in Chinese).
[8]LI Y W,WANG P L,CHEN W W,et al.Formation behavior,microstructure and mechanical properties of multi-cation alpha sialons containing calcium and neodyium[J].Journal of the European Ceramic Society,2001,21(9):1273-1279.
[9]AVCIOGLU S,KURAMA S.Investigation of the influence of initial powder size on the optical properties of Dy-α-SiAlONceramics fabricated by gas pressure sintering[J].Ceramics International,2017,43(s1):449-454.
[10]KHAN R M A,MALKI M M A,HAKEEM A S,et al.Development of a single-phase Ca-α-SiAlON ceramic from nano-sized precursors using spark plasma sintering[J].Materials Science&Engineering A,2016,673:243-249.
[11]YI X M,NIU J,TOMOHIRO A,et al.Spark plasma sintering behavior of combustion synthesized(Y,Ca)-α-SiAlON[J].Ceramics International,2016,42(14):15687-15693.
[12]YANG Z F,WANG H,MIN X M,et al.Translucent Li-α-SiAlON ceramics prepared by spark plasma sintering rapid communications of the American ceramic society[J].Journal of the American Ceramic Society,2010,93(11):3549-3551.
[13]孙洋,陈树江,田琳,等.MgO-sialon/MgO复合材料中Mgsialon片晶的形成和表征[J].复合材料学报,2017,34(3):604-610.SUN Y,CHEN S J,TIAN L,et al.Formation and characterization of Mg-sialon platelet grain in Mg-sialon/MgO composites[J].Acta Materiae Compositae Sinica,2017,34(3):604-610(in Chinese).
[14]YE F,LIU C F,LIU L M.Microstructure and mechanical properties of multi-cation containingα-sialons[J].Ceramics International,2009,35(2):725-731.
[15]刘新,曲殿利,郭玉香,等.自扩散式高温氮化制备Mg-α/β-sialon复相陶瓷[J].人工晶体学报,2016,45(2):435-440.LIU X,QU D L,GUO Y X,et al.Synthesis of Mg-α/β-sialon composites by high temperature self-diffusion nitridation reaction[J].Journal of Synthetic Crystals,2016,45(2):435-440(in Chinese).
[16]桑绍柏,李亚伟,杨纯艳,等.原位反应制备Mg-α-Sialon结合镁质耐火材料研究[J].武汉科技大学学报(自然科学版),2005,28(4):338-342.SANG S B,LI Y W,YANG C Y,et al.Mg-α-Sialon bonded magnesia refractories prepared by in-situ nitridetion process[J].Journal of Wuhan University of Science and Technology(Natural Science Edition),2005,28(4):338-342(in Chinese).
[17]李红霞.耐火原料手册[M].北京:冶金工业出版,2007.LI H X.Manual of refractory materials[M].Beijing:Metallurgical Industry Press,2007(in Chinese).
[18]WANG P L,LI Y W,YAN D S.Effect of amount and atomic ratio of dual modifiers Ca and Mg on phase formation and mechanical properties of Ca,Mg-α-sialons[J].Journal of Materials Science,2000,35(7):1585-1588.
[19]LI Y W,SANG S B,JIN S L,et al.Synthesis of Mg-α-sialon from the mixture of silicon,aluminum and magnesia powders in a flowing nitrogen atmosphere[J].Journal of Materials Science,2006,41(18):5815-5819.
[20]WANG P L,ZHANG C,SUN W Y,et al.Characteristics of Ca-α-sialon phase formation,microstructure and mechanical properties[J].Journal of European Ceramic Society,1999,19(5):553-560.
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