铌酸镁粉体低温合成方法研究进展

doi:10.16552/j.cnki.issn1001-1625.2024.0759

摘要/Abstract

摘要： 铌酸镁微波介质陶瓷因优异的介电性能而备受关注。作为制备高性能铌酸镁陶瓷的关键原料,铌酸镁粉体的质量对最终产品的性能起着至关重要的作用。本文对当前国内外铌酸镁粉体的低温制备方法进行了总结,系统分析了固相反应法、湿化学法、共沉淀法和溶胶凝胶法工艺的优势和局限性,并展望了铌酸镁粉体制备技术的未来发展方向,为高性能铌酸镁粉体材料的研发提供了有益的参考和启示。

关键词: 铌酸镁粉体, 低温合成方法, 固相反应法, 湿化学法, 共沉淀法, 溶胶凝胶法, 微波介质陶瓷

Abstract: Magnesium niobate microwave dielectric ceramics have attracted much attention because of their excellent dielectric properties. Magnesium niobate powder is a crucial raw material for preparing high-performance magnesium niobate ceramics, the quality of which plays a vital role in the performance of final product. In this paper, the current preparation methods of magnesium niobate powder at home and abroad are systematically summarized, the advantages and limitations of solid state reaction method, wet chemical method,co-precipitation method and sol-gel method are analyzed, and the future development direction of magnesium niobate powder preparation technology is prospeced, which provides useful reference and enlightenment for the research and development of high-performance magnesium niobate powder materials.

Key words: magnesium niobate powder, low temperature synthesis method, solid state reaction method, wet chemical method, co-precipitation method, sol-gel method, microwave dielectric ceramics

中图分类号:

TN304

童亚琦, 张微, 李辉, 郑彧, 张杰, 石爽爽. 铌酸镁粉体低温合成方法研究进展[J]. 硅酸盐通报, 2025, 44(1): 305-311.

TONG Yaqi, ZHANG Wei , LI Hui, ZHENG Yu, ZHANG Jie, SHI Shuangshuang. Research Progress on Low Temperature Synthesis Method of Magnesium Niobate Powder[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2025, 44(1): 305-311.

参考文献

[1] WU C H, HU Y D, BAO S X, et al. Microwave dielectric properties of low-temperature-fired MgNb₂O₆ ceramics for LTCC applications[J]. RSC Advances, 2020, 10(50): 29835-29842.
[2] TIAN Z Q, LIN L. Low temperature sintering and microwave dielectric properties of MgNb₂O₆ ceramics[J]. Journal of Materials Science: Materials in Electronics, 2009, 20(9): 867-871.
[3] MAEDA M, YAMAMURA T, IKEDA T. Dielectric characteristics of several complex oxide ceramics at microwave frequencies[J]. Japanese Journal of Applied Physics Supplement, 1987, 26(supplement 2): 76.
[4] 吴承浩. 微波介电陶瓷材料MgNb₂O₆的合成及介电特性研究[D]. 成都: 电子科技大学, 2021.
WU C H. Synthesis and dielectric properties of microwave dielectric ceramic material MgNb₂O₆[D]. Chengdu: University of Electronic Science and Technology of China, 2021 (in Chinese).
[5] SEBASTIAN M T, UBIC R, JANTUNEN H. Low-loss dielectric ceramic materials and their properties[J]. International Materials Reviews, 2015, 60(7): 392-412.
[6] 付志粉, 马建立, 高娟, 等. 高能球磨法制备MgNb₂O₆粉体及其陶瓷性能[J]. 科技导报, 2013, 31(19): 62-65.
FU Z F, MA J L, GAO J, et al. Preparation of MgNb₂O₆ powders by using high-energy ball-milling method and the properties of MgNb₂O₆ ceramics[J]. Science & Technology Review, 2013, 31(19): 62-65 (in Chinese).
[7] WAKINO K, MINAI K, TAMURA H. Microwave characteristics of (Zr, Sn)TiO₄ and BaO-PbO-Nd₂O₃-TiO₂ dielectric resonators[J]. Journal of the American Ceramic Society, 1984, 67(4): 278-281.
[8] 佚名. 新型电子陶瓷材料发展趋势[J]. 人工晶体学报, 2006, 35(1): 205-206.
Anon. Development trend of new electronic ceramic materials[J]. Journal of Synthetic Crystals, 2006, 35(1): 205-206 (in Chinese).
[9] NORIN R, ARBIN C G, NOLANDER B, et al. Note on the phase composition of the MgO-Nb₂O₅ system[J]. Acta Chemica Scandinavica, 1972, 26: 3389-3390.
[10] PAGOLA S, CARBONIO R E, ALONSO J A, et al. Crystal structure refinement of MgNb₂O₆ Columbite from neutron powder diffraction data and study of the ternary system MgO-Nb₂O₅-NbO, with evidence of formation of new reduced pseudobrookiteMg_5-xNb_4+xO_15-δ (1.14≤x≤1.60) phases[J]. Journal of Solid State Chemistry, 1997, 134(1): 76-84.
[11] PULLAR R C. The synthesis, properties, and applications of columbite niobates (M2+Nb₂O₆): a critical review[J]. Journal of the American Ceramic Society, 2009, 92(3): 563-577.
[12] KUMADA N, TAKI K, KINOMURA N. Single crystal structure refinement of a magnesium niobium oxide: Mg₄Nb₂O₉[J]. Materials Research Bulletin, 2000, 35(7): 1017-1021.
[13] YOU Y C, PARK H L, SONG Y G, et al. Stable phases in the MgO-Nb₂O₅ system at 1 250 ℃[J]. Journal of Materials Science Letters, 1994, 13(20): 1487-1489.
[14] ABDUL KHALAM L, THOMAS S, SEBASTIAN M T. Tailoring the microwave dielectric properties of MgNb₂O₆ and Mg₄Nb₂O₉ ceramics[J]. International Journal of Applied Ceramic Technology, 2007, 4(4): 359-366.
[15] WU H T, LI L X, ZOU Q, et al. Synthesis, characterization, and microwave dielectric properties of Mg₄Nb₂O₉ ceramics produced through the aqueous sol-gel process[J]. Journal of Alloys and Compounds, 2011, 509(5): 2232-2237.
[16] WANG H, FU R L, LIU X H, et al. Microstructure and quality factor of Mg₄Nb₂O₉ ceramics via B-site precursor method[J]. Materials Letters, 2021, 293: 129704.
[17] SAHA D, SEN A, MAITI H S. Solid-state synthesis of precursor MgNb₂O₆ for the preparation of Pb(Mg_1/9Nb_2/9)O₉[J]. Journal of Materials Science Letters, 1994, 13(10): 723-724.
[18] SREEDHAR K, MITRA A. Formation of lead magnesium niobate perovskite from MgNb₂O₆ and Pb₃Nb₂O₈ precursors[J]. Materials Research Bulletin, 1997, 32(12): 1643-1649.
[19] YU Y H, FENG C D, LI C G, et al. Formation of columbite-type precursors in the mixture of MgO-Fe₂O₃-Nb₂O₅ and the effects on fabrication of perovskites[J]. Materials Letters, 2001, 51(6): 490-499.
[20] 付志粉, 马建立, 丁兰芳, 等. 高能球磨法低温合成Mg₄Nb₂O₉纳米粉体[J]. 陕西师范大学学报(自然科学版), 2009, 37(6): 23-26.
FU Z F, MA J L, DING L F, et al. Low temperature synthesis of Mg₄Nb₂O₉ nanopowders by high-energy ball-milling method[J]. Journal of Shaanxi Normal University (Natural Science Edition), 2009, 37(6): 23-26 (in Chinese).
[21] SARRAFI M H, BARZEGAR BAFROOEI H, FEIZPOUR M, et al. Microwave synthesis and sintering of Mg₄Nb₂O₉ nanoceramics[J]. Journal of Materials Science: Materials in Electronics, 2014, 25(2): 946-951.
[22] 刘少恒, 杨祖培. 喷雾干燥法制备超细铌酸镁(MgNb₂O₆)粉体[J]. 陕西师范大学学报(自然科学版), 2004, 32(2): 64-67.
LIU S H, YANG Z P. Synthesis of superfine MgNb₂O₆ by spray-drying[J]. Journal of Shaanxi Normal University (Natural Science Edition), 2004, 32(2): 64-67 (in Chinese).
[23] ANANTA S. Phase and morphology evolution of magnesium niobate powders synthesized by solid-state reaction[J]. Materials Letters, 2004, 58(22/23): 2781-2786.
[24] ANANTA S. Synthesis, formation and characterization of Mg₄Nb₂O₉ powders[J]. Materials Letters, 2004, 58(20): 2530-2536.
[25] 苏未安, 边小兵, 刘鹏. Mg₄Nb₂O₉的合成及其微波性能[J]. 硅酸盐通报, 2005, 24(1): 48-50.
SU W A, BIAN X B, LIU P. Synthesis of Mg₄Nb₂O₉ and its microwave property[J]. Bulletin of the Chinese Ceramic Society, 2005, 24(1): 48-50 (in Chinese).
[26] 苏未安, 边小兵, 刘鹏. 温度对Mg₄Nb₂O₉合成的影响[J]. 功能材料, 2004, 35(增刊1): 1240-1242.
SU W A, BIAN X B, LIU P. The influence of temperature on the synthesis of Mg₄Nb₂O₉[J]. Journal of Functional Materials, 2004, 35(supplement 1): 1240-1242 (in Chinese).
[27] 苏靖文, 蒋威, 孟照国, 等. 湿化学法制备ZnO纳米流体[J]. 青岛科技大学学报(自然科学版), 2014, 35(2): 146-151.
SU J W, JIANG W, MENG Z G, et al. ZnO nanofluid synthesized through wet chemical method[J]. Journal of Qingdao University of Science and Technology (Natural Science Edition), 2014, 35(2): 146-151 (in Chinese).
[28] 姚向阳, 芦伟, 纪君宇, 等. 煅烧温度对湿化学法制备AlN粉体的影响[J]. 人工晶体学报, 2022, 51(8): 1451-1458.
YAO X Y, LU W, JI J Y, et al. Effect of calcination temperature on AlN powder prepared by wet chemical method[J]. Journal of Synthetic Crystals, 2022, 51(8): 1451-1458 (in Chinese).
[29] SANTOS L P S, CAMARGO E R, FABBRO M T, et al. Wet-chemical synthesis of magnesium niobate nanoparticles powders[J]. Ceramics International, 2007, 33(7): 1205-1209.
[30] SARKAR K, MUKHERJEE S. Synthesis, characterization and property evaluation of single phase MgNb₂O₆ by chemical route[J]. Journal of the Australian Ceramic Society, 2016, 52(2): 32-40.
[31] SARKAR K, KUMAR V, MUKHERJEE S. Synthesis, characterization and property evaluation of single phase Mg₄Nb₂O₉ by two stage process[J]. Transactions of the Indian Ceramic Society, 2017, 76(1): 43-49.
[32] 王伟, 张启龙, 王焕平, 等. 纳米MgNb₂O₆微波介质陶瓷粉体制备及表征[J]. 无机化学学报, 2006, 22(10): 1887-1890.
WANG W, ZHANG Q L, WANG H P, et al. Preparation and characterization of nano-crystalline MgNb₂O₆ microwave dielectric powder[J]. Chinese Journal of Inorganic Chemistry, 2006, 22(10): 1887-1890 (in Chinese).
[33] 陈元娟. 聚合物前驱体法制备铌酸镁陶瓷的研究[D]. 哈尔滨: 哈尔滨工业大学, 2006.
CHEN Y J. Study on preparation of magnesium niobate ceramics by polymer precursor method[D]. Harbin: Harbin Institute of Technology, 2006 (in Chinese).
[34] 吴兴, 何晓东. MgNb₂O₆陶瓷粉末的共沉淀法制备[J]. 佛山陶瓷, 2020, 30(5): 14-16+39.
WU X, HE X D. Preparation of MgNb₂O₆ ceramic powder by co-precipitation method[J]. Foshan Ceramics, 2020, 30(5): 14-16+39 (in Chinese).
[35] NAVALE S C, GAIKWAD A B, RAVI V. Synthesis of MgNb₂O₆ by coprecipitation[J]. Materials Research Bulletin, 2006, 41(7): 1353-1356.
[36] JOY P A. Low temperature synthesis of Mg₄Nb₂O₉[J]. Materials Letters, 1997, 32(5/6): 347-349.
[37] KAN A, OGAWA H. Low-temperature synthesis and microwave dielectric properties of Mg₄Nb₂O₉ ceramics synthesized by a precipitation method[J]. Journal of Alloys and Compounds, 2004, 364(1/2): 247-249.
[38] GAO Y R, LIU W S, SONG X L, et al. Preparation, characterization and mechanical properties of continuous mullite fibers derived from the diphasic sol-gel route[J]. Journal of Sol-Gel Science and Technology, 2019, 92(1): 75-83.
[39] 马金明, 李佳钰, 陈璐璐, 等. 溶胶-凝胶法制备PbTiO₃纳米粉体[J]. 佛山陶瓷, 2021, 31(10): 10-11+15.
MA J M, LI J Y, CHEN L L, et al. PbTiO₃ nano-size powders obtained by sol-gel process[J]. Foshan Ceramics, 2021, 31(10): 10-11+15 (in Chinese).
[40] OUYANG L F, YANG X J, LI X L, et al. Conductive SrVO₃ powders synthesized by sol-gel method[J]. Science Press, 2022, 51(6): 2039-2044.
[41] PASRICHA R, RAVI V. Preparation of nanocrystalline MgNb₂O₆ by citrate gel method[J]. Materials Letters, 2005, 59(17): 2146-2148.
[42] ZHANG Y C, ZHOU X N, WANG X. Synthesis of MgNb₂O₆ nanocrystalline powders by an improved citrate sol-gel technique[J]. Journal of Sol-Gel Science and Technology, 2009, 50(3): 348-352.
[43] GUO J D, LI C Y, MEI Q J, et al. Effect of MgO excess on structure and microwave dielectric properties of Mg₄Nb₂O₉ ceramics[J]. Materials Technology, 2015, 30(3): 134-137.
[44] HUANG C L, CHIANG K H. Improved high-Q microwave dielectric material using B₂O₃-doped MgNb₂O₆ ceramics[J]. Materials Science and Engineering: A, 2008, 474(1/2): 243-246.
[45] 黄家俊. 铌酸镁基微波介质陶瓷的制备及其性能的优化研究[D]. 景德镇: 景德镇陶瓷大学, 2023.
HUANG J J. Preparation of magnesium niobate-based microwave dielectric ceramics and optimization of their properties[D]. Jingdezhen:Jingdezhen Ceramic University, 2023 (in Chinese).