胺源对“一锅法”合成聚硼硅氮烷结构及性能的影响

陈楚童; 陈艳杰; 罗永明; 张宗波; 徐彩虹

doi:10.11777/j.issn1000-3304.2023.23194

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胺源对“一锅法”合成聚硼硅氮烷结构及性能的影响

研究论文 | 更新时间：2024-01-19

- 胺源对“一锅法”合成聚硼硅氮烷结构及性能的影响
  增强出版
- The Effect of Amine Source on the Structure and Properties of Polyborosilazane Synthesized by "One Pot" Method
- 高分子学报 2024年55卷第2期页码：161-171
- 作者机构：
  
  1.中国科学院化学研究所中国科学院极端环境高分子材料重点实验室北京 100190
  2.中国科学院大学化学与化工学院北京 100049
- 作者简介：
  
  E-mail: luoym@iccas.ac.cn
  zongbo@iccas.ac.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2023.23194
  中图分类号：
- 纸质出版日期：2024-02-20，
  
  网络出版日期：2023-11-22，
  
  收稿日期：2023-09-14，
  
  录用日期：2023-10-07
- 稿件说明：
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陈楚童, 陈艳杰, 罗永明, 张宗波, 徐彩虹. 胺源对“一锅法”合成聚硼硅氮烷结构及性能的影响. 高分子学报, 2024, 55(2), 161-171

Chen, C. T.; Chen, Y. J.; Luo, Y. M.; Zhang, Z. B.; Xu, C. H. The effect of amine source on the structure and properties of polyborosilazane synthesized by "one pot" method. Acta Polymerica Sinica, 2024, 55(2), 161-171
陈楚童, 陈艳杰, 罗永明, 张宗波, 徐彩虹. 胺源对“一锅法”合成聚硼硅氮烷结构及性能的影响. 高分子学报, 2024, 55(2), 161-171 DOI： 10.11777/j.issn1000-3304.2023.23194.

Chen, C. T.; Chen, Y. J.; Luo, Y. M.; Zhang, Z. B.; Xu, C. H. The effect of amine source on the structure and properties of polyborosilazane synthesized by "one pot" method. Acta Polymerica Sinica, 2024, 55(2), 161-171 DOI： 10.11777/j.issn1000-3304.2023.23194.

摘要

以六甲基二硅氮烷(MM

)、四甲基二乙烯基二硅氮烷(MM

NVi

)和四甲基二硅氮烷(MM

) 3种不同结构的二硅氮烷为胺源，通过与氯硅烷和三氯化硼反应，制备出具有不同封端结构的聚硼硅氮烷. 其中，以MM

、MM

NVi

为胺源可获得液态产物；以MM

为胺源时，因合成过程中发生活性基团间的过度交联导致产物凝胶. 采用核磁共振波谱仪、红外光谱仪对液态前驱体聚合物及其热解产物的结构进行了表征. 研究结果表明：通过“一锅法”制备的液态聚硼硅氮烷主链具有较多的支化和环状结构，随着封端结构中乙烯基含量的增加，所得前驱体的固化温度降低，固化反应活化能降低. 与以MM

为胺源和封端剂合成的聚硼硅氮烷相比，以MM

NVi

为胺源所得前驱体固化前后陶瓷产率分别提高了14.9%及8.1%. 并且，通过改变胺源的种类和比例可以调节热解产物的元素组成，合成的液态前驱体聚合物热解所得SiBCN陶瓷结晶温度高于1700 ℃.

Abstract

We used three different structures of disilazane

hexamethyldisilazane (MM

)

tetramethyldivinyldisilazane (MM

NVi

) and tetramethyldisilazane (MM

)

as a source of amine

which then reacted with chlorosilanes and boron trichloride

to produce polyborosilazanes with different end-capped structures. Among the reactants

liquid state products were acquired when using MM

and MM

NVi

as the amine source. While gelatine products were acquired when using MM

as the amine source

due to the excess crosslink of the active group during synthesis. We then used nuclear magnetic resonance spectrometer and infrared spectrometer to characterize the liquid precursor polymer and its pyrolysis products. The results showed that the liquid polyborosilazane backbone made by one pot method had more branches and cyclic structures. As the vinyl group in the end-capped structure increases

the curing temperature of the precursor dropped and the activation energy of the curing reaction lowered. When compared to the polyborosilazane which is made by using MM

and the capping agent

the ceramic production rate increased by 14.9% and 8.1% when MM

NVi

made precursor curation occurred. Furthermore

SiBCN ceramic

made by pyrolysis of the synthetic precursor polymers

has a crystallization temperature higher than 1700 ℃. This conclusion is reached by adjusting the element composition through changing the amine source type and ratio.

关键词

前驱体转化法硅硼碳氮陶瓷聚硼硅氮烷“一锅法”

Keywords

Precursor-derivedSiBCN ceramicPolyborosilazane"One-pot" synthesis

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