有机合成高碳锆比碳化锆陶瓷的先驱体及其热裂解性能
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摘要
以四氯化锆为锆源,苯甲醇为碳源,分别采用对二甲苯,间二甲苯和二甲苯3种不同溶剂,有机合成高碳锆比(原子比28:1)碳化锆陶瓷的先驱体苯甲醇锆(benzyl alcohol zirconium,BAZ)。采用FT-IR对先驱体的基团结构进行表征,通过热重分析(TGA)和X射线衍射分析(XRD)对BAZ的耐热性和陶瓷转化过程进行研究。结果表明,采用不同溶剂制备的碳化锆先驱体在600～700℃时均全部热裂解,1 500℃完全热解为ZrC,其中采用对二甲苯溶剂制备的先驱体在氩气气氛下1 600℃保温1 h后的陶瓷产率最高,为51.8%,采用二甲苯溶剂制备的先驱体热裂解温度最高,为670℃。
Using zirconium tetrachloride as zirconium source,and benzyl methanol as carbon source,precursor benzyl alcohol zirconium(BAZ) of high carbon zirconium ratio(28:1 atomic ratio) zirconium carbide ceramic was prepared by 3 different solvents(p-xylene solvent,m-xylene solvent and xylene solvent).The structure of the BAZ was characterized by FT-IR.The heat-resistant property was studied by TGA and the transformation of ceramic was studied by XRD.The results show that all zirconium carbide precursors prepared by different solvents are pyrolysised during 600-700 ℃ and turn to ZrC after 1 500 ℃ heat treatment.The precursor prepared by p-xylene solvent has the highest ceramic yield of51.8% after 1 600 ℃ heat treatment with argon gas protection.The precursor prepared by xylene solvent has the highest pyrolysis temperature that is 670 ℃.
Using zirconium tetrachloride as zirconium source,and benzyl methanol as carbon source,precursor benzyl alcohol zirconium(BAZ) of high carbon zirconium ratio(28:1 atomic ratio) zirconium carbide ceramic was prepared by 3 different solvents(p-xylene solvent,m-xylene solvent and xylene solvent).The structure of the BAZ was characterized by FT-IR.The heat-resistant property was studied by TGA and the transformation of ceramic was studied by XRD.The results show that all zirconium carbide precursors prepared by different solvents are pyrolysised during 600-700 ℃ and turn to ZrC after 1 500 ℃ heat treatment.The precursor prepared by p-xylene solvent has the highest ceramic yield of51.8% after 1 600 ℃ heat treatment with argon gas protection.The precursor prepared by xylene solvent has the highest pyrolysis temperature that is 670 ℃.
引文
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[3]薛亮,苏哲安,杨鑫,等.先驱体浸渍裂解法制备三维C/C-Hf C复合材料及其烧蚀性能[J].新型炭材料,2017,32(3):265-270.XUE Liang,SU Zhean,YANG Xin,et al.Ablation behavior of a three-dimensional C/C-HfC composite prepared by a precursor infiltration and pyrolysis method[J].New Carbon Materials,2017,32(3):265-270.
[4]刘丹,邱文丰,蔡涛,等.碳化锆液相陶瓷前驱体的制备及陶瓷化[J].宇航材料工艺,2014,44(1):79-83.LIU Dan,QIU Wenfeng,CAI Tao,et al.Preparation and ceramization of liquid Zr C precursor[J].Aerospace Materials&Technology,2014,44(1):79-83.
[5]PIEON D,LUCAS R,CHEHAIDE S,et al.From trimethvlvinylane to Zr C-SiC hybrid materials[J].Eur Ceram Soc,2011,31(14):2687-2690.
[6]WANG H,GAO B,CHEN X,et al.Synthesis and pyrolysis of a novel preceramic polymer PZMS from PMS to fabricate high-temperature-resistant Zr C/SiC ceramic composite[J].Applied Organometallic Chemistry,2013,27(3):166-173.
[7]TANG Y,WANG J,LI X,LI W,et al.Synthesis and characterization of polyborosilazane as novel precursor to SiBNC ceramic[J].Acta Chimica Sinica,2008,66(11):1371-1376.
[8]LI W,WANG J,XIE Z,WANG H,et al.Synthesis and characterization of silicon-containing polyborazine to boron nitride ceramic fiber[J].Acta Chimica Sinica,2011,69(16):1936-1940.
[9]QIN Y,RAO Z,HUANG Z,et al.Preparation and performance of ceramizable heat-resistant organic adhesive for joining Al2O3,ceramics[J].International Journal of Adhesion&Adhesives,2014,55(2):132-138.
[10]BOUZAT F,GRAFF A R,LUCAS R,et al.Preparation of C/SiC ceramics using a preceramic polycarbosilane synthesized via,hydrosilylation[J].Journal of the European Ceramic Society,2016,36(12):2913-2921.
[11]ARISH D,SHIJU C,JOSEYPHUS R S,et al.Synthesis of Zr B2-SiC ceramic composites from a single-source precursor[J].Materials Chemistry&Physics,2017,194:308-312.
[12]PATRA N,NASIRI N A,JAYASEELAN D D,et al.Synthesis,characterization and use of synthesized fine zirconium diboride as an additive for densification of commercial zirconium diboride powder[J].Ceramics International,2016,42(8):9565-9570.
[13]WANG T,YU Q,KONG J,et al.Synthesis and heat-insulating properties of yttria-stabilized Zr O2,hollow fibers derived from a ceiba template[J].Ceramics International,2017.
[14]董占能,赵兵,郭玉忠.金属醇盐的合成(Ⅰ)[J].云南化工,1997(3):58-60.DONG Zhanneng,ZHAO Bing,GUO Yuzhong.Progress in the Synthesis of metal alkoxises[J].Yunnan Chemical Technology,1997(3):58-60.
[15]徐碇皓,高晓梅,周权.含锆耐高温陶瓷化先驱体的合成和性能研究[J].功能材料,2015,46(8):8042-8045.XU Dinghao,GAO Xiaomei,ZHOU Quan.Synthesis and properties of the ceramic precursor containing zirconium and alkyne[J].Journal of Functional Materials,2015,46(8):8042-8045.
[16]董占能,赵兵,郭玉忠.金属醇盐的物化特性[J].昆明理工大学学报:自然科学版,2000,25(2):58-61.DONG Zhanneng,ZHAO Bing,GUO Yuzhong.The pilot study of application of compound fertilizer made of waste mud to paddy[J].Journal of Kunming University Offence&Technology,2000,25(2):58-61.