| 529 | 2 | 222 |
| 下载次数 | 被引频次 | 阅读次数 |
本文从反应机理、Al_2O3–C界面改善技术、高比表面积前驱体制备技术以及反应气氛调控技术诸方面综述了碳热还原氮化(CRN)法合成氮化铝(AlN)粉体的研究进展。依据相关气-固反应讨论了反应过程的质量损失和晶须生长的传质过程，并根据固–固反应控制机理讨论了合成产物与前驱体形貌延续的现象，以及多项研究中Al–O–C与Al–C–N等Al_2O3的转化中间态化合物的形成机制。在固–固反应机理中，C原子因其既能获得电子也能失去电子的性质而充当电子交换媒介促进N2分解和反应正向进行。采用CRN法合成氮化铝粉体技术工艺可归结为：1)通过引入有机高分子分散剂改善C与Al_2O3颗粒的分散态，以形成在原料颗粒尺度层面上的均匀结合界面；2)通过引入黏结剂(如有机碳源)对Al_2O3颗粒均匀包覆，并经热解形成裂解碳与Al_2O3的均匀结合；3)通过有机物分解、燃烧合成、溶胶–凝胶和发泡–注凝等工艺技术实现多孔高比表面积前驱体的制备和铝源与碳源在超微尺度上的均匀混合，进而降低完全反应的条件，以合成纳米AlN粉体；4)增加反应气氛的置换(流动)效率，降低CO分压并增加N2分压以促进合成反应的正向进行。根据现有研究成果，本文还以关键技术与关键装备结合为思路，分别提出发展连续式前驱体制造与连续式高温合成装备，尤其可解决温区差异和气流场差异问题的连续式高温合成装备，以提高CRN法产业化合成AlN粉体性能和效率。
Abstract：This review represents the research progress on the synthesis of aluminium nitride powder via carbon thermal reduction (CRN)in terms of the related reaction mechanism,Al_2O3–C interface improvement,high specific surface area precursor preparation and reaction atmosphere regulation.In this review,the mass loss of the reaction process and the mass transfer process of whisker growth were discussed based on the gas–solid reaction,and the phenomenon of the continuation of the morphology of the synthesized products and precursors as well as the mechanism of the formation of the transformed intermediate state compounds such as Al_2O3 from Al—O—C and Al—C—N were analyzed according to the solid-solid reaction control mechanism.Moreover,the solid-solid reaction mechanism indicates that C atoms act as electron exchange mediators to promote N2 decomposition,and the reaction proceeds in a positive direction due to their ability to both gain and lose electrons.Recent research work on the CRN method for the synthesis of AlN powder was summarized.Summary and prospects These researches involve 1) the introduction of organic dispersants to increase the dispersion of C and Al_2O3 particles,and the formation of a uniform binding interface between particles,2) the introduction of a binder (i.e.,an organic carbon source) on the uniform coating of Al_2O3 particles and pyrolysis to form a uniform combination of cracked carbon and Al_2O3 particles,3) the decomposition of organic matter,combustion synthesis and sol–gel and foam-injection coagulation to obtain precursors with a porous structure and a high specific surface area and the uniform mixing of aluminium and carbon sources in a micron scale,thus reducing the conditions for complete reaction and synthesizes high-quality nanopowders of AlN and 4) increasing the substitution (flow) efficiency of the reaction atmosphere,reducing the partial pressure of CO and increasing the partial pressure of N2 to promote the positive synthesis reaction.According to the existing research,the future industrial development can be based on the combination of key process technology and key equipment.The continuous precursor manufacturing and continuous high-temperature synthesis equipment,especially continuous high-temperature synthesis equipment to eliminate differences in temperature zones and in airflow fields,need to be developed for the enhanced performance and efficiency of AlN powder synthesized by the CRN method.
[1] WEI X, ZHANG H, DANG J J, et al. Effects of grain boundary phase distributions on mechanical characteristics of the high thermal conductivity AlN ceramics[J]. Ceram Int, 2024, 50(17):29632–29641.
[2] JIANG H, WANG X H, LEI W, et al. Effects of two-step sintering on thermal and mechanical properties of aluminum nitride ceramics by impedance spectroscopy analysis[J]. J Eur Ceram Soc, 2019, 39(2/3):249–254.
[3] KIM J I, KIM J, LEE S M, et al. Low-temperature hot-press sintering of AlN ceramics with MgO–CaO–Al2O3–SiO2 glass additives for ceramic heater applications[J]. Ceram Int, 2022, 48(18):26022–26027.
[4]朱亚军,王国栋,俞瑞仙,等.物理气相传输法SiC衬底上生长AlN单晶的研究进展[J].硅酸盐学报, 2023, 51(6):1439–1449.ZHU Yajun, WANG Guodong, YU Ruixian, et al. J Chin Ceram Soc,2023, 51(6):1439–1449..
[5]何端鹏,黄雪吟,任刚等.高热导电绝缘氮化铝陶瓷在宇航器件中的应用：概述、挑战和展望[J].硅酸盐学报, 2022, 50(6):1701–1714.HE Duanpeng, HUANG Xueyin, REN Gang, et al. J Chin Ceram Soc,2022, 50(6):1701–1714.
[6] LU C Y, ZHANG C Y, XU H T, et al. Constructing a heterogeneous interlayer in relieving the residual stresses for the AlN/Cu brazed joint used in IGBT[J]. Mater Charact, 2023, 199:112759.
[7] LEI D, HAN K Z, WU Y, et al. High performance Ga2O3metal–oxide–semiconductor field-effect transistors on an AlN/Si substrate[J]. IEEE J Electron Devices Soc, 2019, 7:596–600.
[8] JEONG J S, AN Y G. Lifetime and degradation analysis of AgPt alloy thick film/AlN heater for semiconductor wafer annealing[J].Microelectron Reliab, 2021, 126:114402.
[9] FU R, CHEN K, AGATHOPOULOS S, et al. Factors which affect the morphology of AlN particles made by self-propagating high-temperature synthesis(SHS)[J]. J Cryst Growth, 2006, 296(1):97–103.
[10]侯海兰,冯月斌,字富庭,等.碳热还原氮化法制备氮化铝的研究进展[J].粉末冶金工业, 2019, 29(1):69–72.HOU Hailan, FENG Yuebin, ZI Futing, et al. Powder Metall Ind, 2019,29(1):69–72.
[11]张智睿,秦明礼,吴昊阳,等.氮化铝粉末制备方法及研究进展[J].粉末冶金技术, 2021, 39(4):373–382.ZHANG Zhirui, QIN Mingli, WU Haoyang, et al. Powder Metall Technol, 2021, 39(4):373–382.
[12] LEFORT P, BILLY M. Mechanism of AlN formation through the carbothermal reduction of Al2O3 in a flowing N2 atmosphere[J]. J Am Ceram Soc, 1993, 76(9):2295–2299.
[13] HIRAI S, MIWA T, IWATA T, et al. Formation of AlN by carbothermic reduction of Al2O3 in a flowing N2 atmosphere[J]. JPn Inst Metals,1989, 53(10):1035–1040.
[14] FORSLUND B, ZHENG J. Carbothermal synthesis of aluminium nitride at elevated nitrogen pressures:Part II Effect of process parameters on particle size and morphology[J]. J Mater Sci, 1993,28(12):3132–3136.
[15]张笑.氧化铝碳热还原氮化的机理研究[D].昆明:昆明理工大学,2017.ZHANG Xiao. Study on mechanism of carbothermal reduction nitridation of alumina[D]. Kunming:Kunming University of Science and Technology, 2017.
[16]黄莉萍,黄熊璋,符锡仁,等.氮化铝粉末的制备[J].硅酸盐学报,1986(3):78–84, 135.HUANG Liping, HUANG Xingzhang, FU Xiren, et al. J Chin Ceram Soc, 1986(3):78–84, 135.
[17] O’DONNELL R G, TRIGG M B. The mechanism of conversion of Al2O3 to Al N via carbothermal synthesis[J]. Micron, 1994, 25(6):575–579.
[18] ZHOU Z Q, XU Y L, CHEN X M, et al. Preparation of AlN under vacuum by the alumina carbothermal reduction nitridation method[J].Ceram Int, 2020, 46(4):4095–4103.
[19] ZHOU Z Q, CHEN X M, ZHAO Z Q, et al. Ab initio and experimental study of the mechanism of alumina carbothermal reduction and nitridation under vacuum[J]. Ceram Int, 2021, 47(19):27972–27978.
[20] XU Y L, ZHOU Z Q, CHEN X M, et al. Ultrafine AlN synthesis by alumina carbothermal reduction under vacuum:Mechanism and experimental study[J]. Powder Technol, 2021, 377:843–846.
[21] HE B Y, CHEN X M, DENG P, et al. Ab initio and experimental study on the mechanism of Al4C3 nitridation in vacuum to prepare AlN[J].Ceram Int, 2022, 48(5):6977–6984.
[22] Kang M S, Shin K H, Kim D W, et al. Optimisation study for making aluminium nitride using an improved carbothermal reductionnitridation process[J]. J Ceram Process Res, 2017, 18(12):848–853.
[23] SUN X N, WANG J B, WANG Z C, et al. Preparation of single phase nano-sized AlN powder by carbothermal reduction and nitridation of hydrothermal synthesized carbon coated γ-Al2O3 from glucose via fast heating[J]. Ceram Int, 2023, 49(13):22128–22138.
[24] WANG L Y, ZHANG N. Mechanism and research on preparation of AlN powder by carbon thermal reduction method[J]. IOP Conf Ser:Mater Sci Eng, 2019, 647(1):012007.
[25]翁履谦,黄栋生,黄尚文.碳热法合成AIN的热力学及动力学[J].硅酸盐通报, 1993(5):29–31, 37.WENG lvqian, HUANG Dongsheng, HUANG Shangwen, Bull Chin Ceram Soc, 1993(5):29–31, 37.
[26] WANG Y M, QIAO L, ZHENG J W, et al. Preparation of AlN with low agglomeration using polyethylene glycol and emulsifier to disperse the ultrafine raw powders[J]. Ceram Int, 2023, 49(1):1390–1400.
[27]温倩.碳热还原氮化法制备低团聚氮化铝陶瓷粉体的研究[D].杭州:浙江工业大学, 2021.WEN Qian. Study on preparation of low agglomeration aluminum nitride ceramic powder by carbothermal reduction nitridation[D]. Hangzhou:Zhejiang University of Technology, 2021.
[28] WEN Q, WANG P, ZHENG J W, et al. Carbothermal reduction synthesis of aluminum nitride from Al(OH)3/C/PVB slurries prepared by three-roll mixing[J]. Materials, 2021, 14(6):1386.
[29] JUNG W S, AHN S K. Preparation of aluminium nitride powder from a(hydroxo)(succinato)aluminium(III)complex[J]. J Mater Chem, 1994,4(6):949–953.
[30] AHN S K, OH C W, JUNG W S. Conversion of succinateand adipate-coordinated Al(III)complexes to AlN in N2 and NH3atmospheres[J]. J Korean Ceram Soc, 1996, 33(4):455–463.
[31] JUNG W S, AHN S K. Synthesis of aluminum nitride by a modified carbothermal reduction and nitridation method using basic dicarboxylate Al(III)complexes Al(OH)(Cn+2H2nO4)·x H2O(n=3, 6,8)[J]. J Eur Ceram Soc, 2001, 21(1):79–85.
[32] XIANG M, ZHOU Y F, XU W T, et al. Hydrothermal-carbothermal synthesis of highly sinterable AlN nanopowders[J]. J Am Ceram Soc,2017, 100(6):2482–2491.
[33]魏鑫,张浩,孙登琼,等.碳热还原氮化法制备超细AlN粉体的过程及特性[J].粉末冶金材料科学与工程, 2018, 23(6):624–631.WEI Xin, ZHANG Hao, SUN Dengqiong, et al. Mater Sci Eng Powder Metall, 2018, 23(6):624–631.
[34] MYLINH D T, YOON D H, KIM C Y. Aluminum nitride formation from aluminum oxide/phenol resin solid–gel mixture by carbothermal reduction nitridation method[J]. Arch Metall Mater, 2015, 60(2):1551–1555.
[35] FUMO D A, JURADO J, SEGAD?ES A M, et al. Combustion synthesis of iron-substituted strontium titanate perovskites[J]. Mater Res Bull, 1997, 32(10):1459–1470.
[36]秦明礼,曲选辉,肖平安,等.尿素对前驱物及氮化铝粉末粒度形貌的影响[J].粉末冶金材料科学与工程, 2002, 7(4):277–282.QIN Mingli, QU Xuanhui, XIAO Ping’an, et al. Mater Sci Eng Powder Metall, 2002, 7(4):277–282.
[37] CHU A M, QIN M L, RAFI-UD-DIN, et al. Effect of urea on the size and morphology of AlN nanoparticles synthesized from combustion synthesis precursors[J]. J Alloys Compd, 2012, 530:144–151.
[38] PATHAK L C, RAY A K, DAS S, et al. Carbothermal synthesis of nanocrystalline aluminum nitride powders[J]. J Am Ceram Soc, 1999,82(1):257–260.
[39] CHU A M, QIN M L, RAFI-UD-DIN, et al. Citric acid-assisted combustion-carbothermal synthesis of well-distributed highly sinterable AlN nanopowders[J]. J Am Ceram Soc, 2012, 95(8):2510–2515.
[40] CHU A M, ZHAO Y P, UD-DIN R, et al. Carbon-containing droplet combustion-carbothermal synthesis of well-distributed AlN nanometer powders[J]. J Am Ceram Soc, 2022, 105(10):5999–6006.
[41]秦明礼,曲选辉,林健凉,等.低温碳热还原法合成氮化铝陶瓷超细粉末[J].无机材料学报, 2002, 17(5):1054–1058.QIN Mingli, QU Xuanhui, LIN Jianliang, et al. J Inorg Mater, 2002,17(5):1054–1058.
[42]仝建峰,周洋,陈大明.氮化铝粉末的制备方法与机理[J].硅酸盐通报, 2002, 21(5):12–16.TONG Jianfeng, ZHOU Yang, CHEN Daming. Bull Chin Ceram Soc,2002, 21(5):12–16.
[43]秦明礼,曲选辉,林健凉,等.溶胶–凝胶工艺制备氮化铝陶瓷超细粉末[J].粉末冶金材料科学与工程, 2002, 7(1):50–54.QIN Mingli, QU Xuanhui, LIN Jianliang, et al. Mater Sci Eng Powder Metall, 2002, 7(1):50–54.
[44]张璞,杨金萍,魏恒勇,等.非水解溶胶–凝胶结合碳热还原氮化法制备AIN粉体工艺研究[J].中国陶瓷, 2014, 50(7):33–36.ZHANG Pu, YANG Jinping, WEI Hengyong, et al. China Ceram, 2014,50(7):33–36.
[45]魏颖娜,魏恒勇,赵冬梅,等.基于非水解sol–gel法的碳热还原氮化合成氮化铝超细粉体[J].功能材料, 2013, 44(17):2546–2549.WEI Yingna, WEI Hengyong, ZHAO Dongmei, et al. J Funct Mater,2013, 44(17):2546–2549.
[46] MAO X X, LI J, ZHANG H L, et al. Synthesis of Al N powder by carbothermal reduction-nitridation of alumina/carbon black foam[J]. J Inorg Mater, 2017, 32(10):1115–1120.
[47] MAO X X, XU Y G, MAO X J, et al. Synthesis of fine AlN powders by foamed precursor-assisted carbothermal reduction-nitridation method[J].J Inorg Mater, 2019, 34(10):1123–1127.
[48] CANIKO?LU N. Synthesizing of nano-sized AlN powder with alumina balls[J]. J Ceram Process Res, 2021, 22(3):258–263.
[49] BOUSSEBHA H, MUTLU N, CANIKO?LU N, et al. Synthesis of submicron AlN powder using dynamic/thermochemical method[J]. Int J Appl Ceram Technol, 2022, 19(6):2967–2978.
[50] FORSLUND B, ZHENG J. Carbothermal synthesis of aluminium nitride at elevated nitrogen pressures:Part I Effect of process parameters on conversion rate[J]. J Mater Sci, 1993, 28(12):3125–3131.
[51] SHAN C, XU J H, SUN X N, et al. Preparation of AlN powder of low oxygen content via carbothermal reduction and nitridation by active gas exchange technique[J]. Ceram Int, 2020, 46(13):21182–21189.
基本信息:
DOI：10.14062/j.issn.0454-5648.20240399
中图分类号:TQ133.1
引用信息:
[1]袁振侠,李大海,徐佳豪,等.碳热还原氮化法制备氮化铝粉体研究进展[J].硅酸盐学报,2024,52(12):3884-3895.DOI:10.14062/j.issn.0454-5648.20240399.
基金信息:
国家自然科学基金(U23A20562); 宁夏重点研发专项(2023BDE92008); 银川市科技创新领军人才培养工程(2023LJRC08)资助; 银川市科技计划项目(2023GXZD17)
2024-11-15
2024-11-15
2024-11-15