SiBN三元陶瓷纤维的聚硼硅氮烷裂解转化制备和性能
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摘要
以三氯硅烷、六甲基二硅氮烷、三氯化硼和甲胺为原料合成聚硼硅氮烷前驱体,对前驱体进行熔融纺丝和不熔化处理,将其高温裂解后制备出SiBN陶瓷纤维。使用FT-IR、NMR、XRD、TEM、TGA等表征手段研究了在不同聚合温度下聚硼硅氮烷前驱体的化学结构特征、SiBN陶瓷纤维的高温热稳定性、介电性能以及力学性能。结果表明:在不同温度下制备的聚硼硅氮烷前驱体的骨架为Si-N-B,均含有HSiN3、BN3及NCH3等结构。在1400℃热处理后SiBN陶瓷纤维仍保持无定形态,直径为14μm,拉伸强度达到0.91 GPa。在氮气气氛中SiBN陶瓷纤维从室温到1400℃的失重为1.5%,表明这种纤维具有较高的热稳定性。SiBN陶瓷纤维的介电常数为2.6～2.8,损耗角正切的数量级为10-2。
Polyborosiliazne precursor was synthesized via multi-stage polymerization process with HSiCl_3, Me_6Si_2NH, BCl_3 and CH_3NH_2 as raw materials. Then SiBN ceramic fibers were obtained by melt spinning, curing and pyrolysis of the as-synthesized polyborosilazane precursor. The chemical structure,high temperature thermal stability, dielectric property and mechanical property of the polyborosilazane and its pyrolysis products were investigated by FT-IR, NMR, XRD, TEM and TGA. FT-IR and NMR. Results show that the polyborosilazane precursors prepared at different temperatures exhibited similar chemical structures, namely, containing Si-N, B-N and N-CH3 bonds. The obtained SiBN ceramic fibers remained amorphous structure with 14 μm in diameter and 0.91 GPa in tensile strength after heat treatment at 1400 oC. The SiBN ceramic fibers have excellent thermal stability with only 1.5% mass loss in the temperature range from room temperature to 1400 oC. The dielectric constant and dielectric loss loss tangent magnitude of SiBN ceramic fibers are 2.6～2.8 and 10-2 at 1100 oC, respectively.
Polyborosiliazne precursor was synthesized via multi-stage polymerization process with HSiCl_3, Me_6Si_2NH, BCl_3 and CH_3NH_2 as raw materials. Then SiBN ceramic fibers were obtained by melt spinning, curing and pyrolysis of the as-synthesized polyborosilazane precursor. The chemical structure,high temperature thermal stability, dielectric property and mechanical property of the polyborosilazane and its pyrolysis products were investigated by FT-IR, NMR, XRD, TEM and TGA. FT-IR and NMR. Results show that the polyborosilazane precursors prepared at different temperatures exhibited similar chemical structures, namely, containing Si-N, B-N and N-CH3 bonds. The obtained SiBN ceramic fibers remained amorphous structure with 14 μm in diameter and 0.91 GPa in tensile strength after heat treatment at 1400 oC. The SiBN ceramic fibers have excellent thermal stability with only 1.5% mass loss in the temperature range from room temperature to 1400 oC. The dielectric constant and dielectric loss loss tangent magnitude of SiBN ceramic fibers are 2.6～2.8 and 10-2 at 1100 oC, respectively.
引文
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[2]Hannemann A,Sch?n J C,Jansen M,et al.Nonequilibrium dynamics in amorphous Si3B3N7[J].J.Phys.Chem.,2005,109B:11770
[3]Ji X Y,Wang S S,Shao C W,et al.High-temperature corrosion behavior of SiBCN fibers for aerospace applications[J].ACS Appl.Mater.Interfaces,2018,10:19712
[4]Tang Y,Wang J,Li X D,et al.Performance of polyborosilazane and SiBNC ceramics thereof[J].Chin.J.Mater.Res.,2008,22:291(唐云,王军,李效东等.聚硼硅氮烷先驱体的合成及其目标陶瓷SiBNC的性能[J].材料研究学报,2008,22:291)
[5]Liu Y,Chen K Z,Dong F B,et al.Effects of hydrolysis of precursor on the structures and properties of polymer-derived SiBN ceramic fibers[J].Ceram.Int.,2018,44:10199
[6]Van Wüllen L,Jansen M.The role of carbon in the nitridic high performance ceramics in the system Si-B-N-C[J].Solid State Nucl.Magn.Reson.,2005,27:90
[7]J?schke T,Jansen M.Synthesis and characterization of new amorphous Si/B/N/C ceramics with increased carbon content through single-source precursors[J].C.R.Chim.,2004,7:471
[8]J?schke T,Jansen M.Improved durability of Si/B/N/C random inorganic networks[J].J.Eur.Ceram.Soc.,2005,25:211
[9]Tang Y,Wang J,Li X D,et al.Polymer-derived SiBN fiber for high-temperature structural/functional applications[J].Chem.Eur.J.,2010,16:6458
[10]Yuan J,Han K Q,Zhao X,et al.Melt spinning process and characterization of precursors for SiBN(C)ceramic fiber[J].Chin.Syn.Fiber Ind.,2011,34:1(袁佳,韩克清,赵曦等.SiBN(C)陶瓷纤维先驱体的表征及熔融纺丝[J].合成纤维工业,2011,34:1)
[11]Colombo P,Mera G,Riedel R,et al.Polymer-derived ceramics:40years of research and innovation in advanced ceramics[J].J.Am.Ceram.Soc.,2010,93:1805
[12]Ge K K,Ye L,Han W J,et al.Pyrolysis of polyborosilazane and its conversion into SiBN ceramic[J].Adv.Appl.Ceram.,2014,113:367
[13]Tang Y,Wang J,Li X D,et al.Preparation of high performance SiB-N ceramic fibers by polymer derived method[J].Acta Chim.Sin.,2009,67:2750(唐云,王军,李效东等.先驱体转化法制备高性能Si-B-N陶瓷纤维[J].化学学报,2009,67:2750)
[14]Tang Y,Wang J,Li X D,et al.Preceramic polymer for Si-B-N-Cfiber via one-step condensation of silane,BCl3,and Silazane[J].J.Appl.Polym.Sci.,2008,110:921
[15]Li W H,Wang J,Xie Z F,et al.Preparation of hollow Si-B-N ceramic fibers by partial curing and pyrolysis of polyborosilazane fibers[J].Mater.Lett.,2012,78:1
[16]Peng Y Q,Han K Q,Zhao X,et al.Large-scale preparation of SiBN ceramic fibres from a single source precursor[J].Ceram.Int.,2014,40:4797
[17]Funayama O,Nakahara H,Okoda M,et al.Conversion mechanism of polyborosilazane into silicon nitride-based ceramics[J].J.Mater.Sci.,1995,30:410
[18]Funayama O,Kato T,Tashiro Y,et al.Synthesis of a polyborosilazane and its conversion into inorganic compounds[J].J.Am.Ceram.Soc.,1993,76:717
[19]Wideman T,Fazen P J,Su K,et al.Second-generation polymeric precursors for BN and SiNCB ceramic materials[J].Appl.Organomet.Chem.,1998,12:681
[20]Wideman T,Cortez E,Remsen E E,et al.Reactions of monofunctional boranes with hydridopolysilazane:synthesis,characterization,and ceramic conversion reactions of new processible precursors to SiNCB ceramic materials[J].Chem.Mater.,1997,9:2218
[21]Mou S W,Hu J J,Wang H F,et al.Structure and rheological property of polyborosilazane[J].J.Mater.Sci.Eng.,2016,34:63(牟世伟,胡建建,王会峰等.SiBNC陶瓷纤维前驱体的结构及流变性能[J].材料科学与工程学报,2016,34:63)
[22]Huang X H,Liu Y,Zhang C Y,et al.Decarburization research of SiBN ceramic fibers[J].Chin.Syn.Fiber Ind.,2017,40:1(黄先华,刘勇,张晨宇等.SiBN陶瓷纤维的脱碳工艺研究[J].合成纤维工业,2017,40:1)
[23]Gervais C,Babonneau F,Ruwisch L,et al.Solid-state NMR investigations of the polymer route to SiBCN ceramics[J].Can.J.Chem.,2003,81:1359
[24]Liu Y,Peng S,Cui Y J,et al.Fabrication and properties of precursor-derived SiBN ternary ceramic fibers[J].Mater.Des.,2017,128:150
[25]Schuhmacher J,Berger F,Weinmann M,et al.Solid-state NMRand FT IR studies of the preparation of Si-B-C-N ceramics from boron-modified polysilazanes[J].Appl.Organomet.Chem.,2001,15:809
[26]Cheng F,Toury B,Archibald S J,et al.Synthesis and structure of2,4,6-tris[tris(dimethylamino)silylamino]borazine:{[(CH3)2N]3-SiNH}3B3N3H3[J].J.Organomet.Chem.,2002,657:71