SiBN三元陶瓷纤维的聚硼硅氮烷裂解转化制备和性能

doi:10.11901/1005.3093.2018.373

材料研究学报

2019, Vol. 33

Issue (2): 155-160 DOI: 10.11901/1005.3093.2018.373

本期目录 | 过刊浏览

SiBN三元陶瓷纤维的聚硼硅氮烷裂解转化制备和性能

崔永杰,刘勇(

),彭帅,韩克清,余木火

纤维材料改性国家重点实验室东华大学材料科学与工程学院上海 201620

Preparation and Property of SiBN Ternary Ceramic Fibers Prepared by Polyborosilazane-Derived Method

Yongjie CUI,Yong LIU(

),Shuai PENG,Keqing HAN,Muhuo YU

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China

引用本文:

崔永杰,刘勇,彭帅,韩克清,余木火. SiBN三元陶瓷纤维的聚硼硅氮烷裂解转化制备和性能[J]. 材料研究学报, 2019, 33(2): 155-160.
Yongjie CUI, Yong LIU, Shuai PENG, Keqing HAN, Muhuo YU. Preparation and Property of SiBN Ternary Ceramic Fibers Prepared by Polyborosilazane-Derived Method[J]. Chinese Journal of Materials Research, 2019, 33(2): 155-160.

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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14 μm，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。

关键词 ：无机非金属材料, 聚硼硅氮烷, 高温裂解, SiBN陶瓷纤维, 热稳定性, 介电性能

Abstract：

Polyborosiliazne precursor was synthesized via multi-stage polymerization process with HSiCl₃, Me₆Si₂NH, BCl₃ and CH₃NH₂ 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.

Key words： inorganic nonmetallic materials polyborosilazane pyrolysis SiBN ceramic fiber thermal stability dielectric property

收稿日期: 2018-06-06

ZTFLH:

TQ343

基金资助:国家自然科学基金(51703025)

作者简介: 崔永杰，男，1994年生，硕士生

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https://www.cjmr.org/CN/10.11901/1005.3093.2018.373 或 https://www.cjmr.org/CN/Y2019/V33/I2/155

图1 不同聚合温度制备的PBSZ前驱体的FT-IR谱

图2 在不同温度聚合制备的PBSZ前驱体的13C-MAS NMR谱

图3 不同聚合温度制备的PBSZ前驱体的29Si-MAS NMR谱

图4 不同聚合温度制备的PBSZ前驱体的11B-NMR谱图

图5 PBSZ前驱体的制备反应过程

图6 不同温度裂解得到的SiBN陶瓷纤维的XRD谱

图7 1400℃裂解得到的SiBN陶瓷纤维的TEM照片

图8 SiBN陶瓷纤维的TGA曲线(N2气氛)

图9 SiBN陶瓷纤维介电常数和损耗角正切值随裂解温度的变化

表1 PBSZ初生纤维、不熔化纤维及不同裂解温度得到的SiBN纤维的力学性能

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