基于外场作用的SEBS形态演变对PPS基复合材料力学性能的影响

易成鸿; 谢林生; 吉华建; 李果; 马玉录; 王玉

基于外场作用的SEBS形态演变对PPS基复合材料力学性能的影响

华东理工大学　机械与动力工程学院

详细信息

通讯作者:
王　玉，博士，助理研究员，研究方向为过程装备及材料加工　E-mail: wangyu_ecust@ecust.edu.cn

中图分类号: TB332
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出版历程
- 收稿日期: 2023-12-05
- 修回日期: 2024-01-07
- 录用日期: 2024-02-03
- 网络出版日期: 2024-03-12

Impact of the morphological evolution of SEBS based on external field effects on the mechanical properties of PPS composite materials

School of Mechanical and Power Engineering, East China University of Science and Technology

摘要

摘要: 聚苯硫醚(PPS)是一种热塑性工程材料，具有强度高、稳定性好等优点，现已在国防、民用领域得到广泛的应用。然而PPS本身的韧性较差，通常通过添加弹性体进行增韧改性以扩大其应用范围。本研究基于高拉伸混沌流的混炼转子，通过熔融共混法制备了氢化苯乙烯-丁二烯嵌段共聚物/聚苯硫醚(SEBS/PPS)复合材料，研究了不同含量SEBS在高拉伸外场作用下的微观形态演变行为，分析了其对PPS基复合材料力学性能的影响规律。结果表明：随着SEBS含量的增加，PPS基复合材料的冲击强度和断裂伸长率呈现先增加后下降的趋势；当SEBS含量达到6wt%时，复合材料呈现韧性断裂行为，其冲击强度和断裂伸长率达到最高，分别为67.8J/m和6.1%。通过对复合材料微观结构分析发现：在高拉伸混炼转子作用下，当SEBS含量在0~6wt%之间时，SEBS粒径尺寸较小，分布均匀，液滴形态向拉伸棒状演变，此时复合材料发生脆韧转变，韧性明显增强，且在6wt% SEBS含量的复合材料受到冲击力时引发多重银纹，发生剪切屈服，表现为塑性变形；当SEBS含量继续增加时，其团聚行为加剧，粒径尺寸随之逐渐增加，且分布较宽，同时两相界面出现大量空穴区域，在引发银纹发展的同时也会导致复合材料的断裂失效，使得复合材料冲击强度有所下降。
- 聚苯硫醚 /
- 氢化苯乙烯-丁二烯嵌段共聚物 /
- 力学性能 /
- 微观结构 /
- 增韧机制
Abstract: Polyphenylene sulfide (PPS) stands as a thermoplastic engineering material, renowned for its high strength and excellent stability. It has found extensive applications in both defense and civilian sectors. However, the intrinsic lack of toughness in PPS necessitates toughness enhancement for broadening its application scope, typically achieved through the incorporation of elastomers. In this study, a melt-blending technique utilizing a high-stretch chaotic flow rotor was employed to prepare hydrogenated styrene-butadiene-styrene block copolymer/polyphenylene sulfide (SEBS/PPS) composite materials. The research aimed to investigate the microstructural evolution of the materials under the influence of high-stretch external forces and analyze the impact of varying SEBS content on the mechanical properties of the PPS-based composite materials. The results indicate that with an increase in SEBS content, the impact strength and fracture elongation of the PPS-based composite materials exhibit an initial rise followed by a subsequent decline. When the SEBS content reaches 6wt%, the composite material demonstrates a ductile fracture behavior, achieving the highest impact strength and fracture elongation at 67.8 J/m and 6.1%, respectively. Microstructural analysis of the composite material reveals that within the SEBS content range of 0~6wt%, under the action of the high-stretch blending rotor, SEBS particles exhibit smaller and more uniformly distributed sizes. The droplet morphology undergoes a transition to elongated rod shapes, indicating a brittle-to-ductile transformation and a significant improvement in toughness. In the composite material with 6wt% SEBS content, multiple silver streaks are induced upon impact, leading to shear yielding and exhibiting plastic deformation. Continued increase in SEBS content intensifies the aggregation behavior of SEBS, resulting in an enlargement of particle sizes and broader distribution. At this stage, numerous void regions appear at the two-phase interfaces, triggering the development of silver streaks and concurrently causing fracture failure in the composite material, leading to a decrease in impact strength.
- Polyphenylene sulfide /
- Hydrogenated styrene-butadiene block copolymer /
- Mechanical properties /
- Microstructure /
- Toughening mechanism

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图 1 双转子连续混炼挤出机的转子结构

Figure 1. Rotor structure of two-rotor continuous mixing extruder

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图 2 不同SEBS含量的氢化苯乙烯-丁二烯嵌段共聚物/聚苯硫醚(SEBS/PPS)复合材料的力学性能：(a) 冲击强度；(b) 断裂伸长率；(c) 拉伸性能；(d) 弯曲性能

Figure 2. Mechanical properties of SEBS/PPS composites with different hydrogenated styrene-butadiene-styrene block copolymer/polyphenylene sulfide (SEBS/PPS) contents: (a) Impact strength; (b) Elongation at break; (c) Tensile properties; (d) Bending properties

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图 3 不同SEBS含量的SEBS/PPS复合材料拉伸性能测试时的应力应变曲线及破坏试样图片： (a) 应力应变曲线；(b) 拉伸破坏试样；(c) 冲击破坏试样

Figure 3. Stress-strain curves and sample images during tensile performance testing of SEBS/PPS composites with different SEBS contents: (a) Stress-strain curves; (b) Tensile failure samples; (c) Impact failure samples

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图 4 不同SEBS含量的SEBS/PPS复合材料的动态力学性能：(a) 储能模量 (b) 损耗模量(c) 损耗角正切值

Figure 4. Dynamic mechanical properties of SEBS/PPS composites with different SEBS contents: (a) Storage modulus (b) Loss modulus (c) Loss angle tangent

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图 5 不同SEBS含量的SEBS/PPS复合材料的SEM照片：SEBS含量：(a) 0 % (b) 3wt% (c) 6wt % (d) 9wt% (e) 15wt% (f) 20wt%

Figure 5. SEM photographs of SEBS/PPS composites with different SEBS contents: content of SEBS /wt%: (a) 0 % (b) 3wt% (c) 6wt % (d) 9wt% (e) 15wt% (f) 20wt%

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图 6 不同SEBS含量的SEBS/PPS复合材料的DSC曲线:(a) 熔融曲线 (b) 结晶曲线(1-0wt%SEBS; 2-3wt% SEBS; 3-6wt% SEBS; 4-9wt% SEBS; 5-15wt% SEBS; 6-20wt% SEBS)

Figure 6. DSC curves of SEBS/PPS composites with different SEBS contents: (a) Melt curve (b) Crystallization curve (1-0wt%SEBS; 2-3wt% SEBS; 3-6wt% SEBS; 4-9wt% SEBS; 5-15wt% SEBS; 6-20wt% SEBS)

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图 7 不同SEBS含量的SEBS/PPS复合材料冲击断面SEM照片：SEBS含量:(a) 0 % (b) 3wt% (c) 6 wt % (d) 9wt% (e) 15wt% (f) 20wt%

Figure 7. SEM images of impact sections of SEBS/PPS composites with different SEBS contents: content of SEBS: (a) 0 % (b) 3wt% (c) 6 wt % (d) 9wt% (e) 15wt% (f) 20wt%

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图 8 不同SEBS含量的SEBS/PPS复合材料的冲击断面TEM照片：SEBS含量:(a) 3wt% (b) 6wt% (c) 20wt%

Figure 8. TEM images of impact sections of SEBS/PPS composites with different SEBS contents: content of SEBS:(a) 3wt% (b) 6wt% (c) 20wt%

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图 9 SBES/ PPS的复合材料增韧模型: SEBS含量: (a) 3wt% (b) 6wt% (c) 20wt%

Figure 9. Toughening model of composites with SBES/ PPS: content of SEBS: (a) 3wt% (b) 6wt% (c) 20wt%

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表 1 不同SEBS含量的SEBS/PPS复合材料动态力学性能数据

Table 1. Data on dynamic mechanical properties of SEBS/PPS composites with different SEBS contents

Content of SEBS /wt%	Storage modulus /MPa		T_g1/℃	T_g2/℃	ΔT_g
Content of SEBS /wt%	−50℃	50℃	T_g1/℃	T_g2/℃	ΔT_g
0	2254.2	2131.7	/	124.69	/
3	2576.6	2382.1	4.38	127.19	122.81
6	2761.6	2561.2	4.80	125.35	120.55
9	2465.6	2217.9	4.02	126.12	122.10
15	2750.31	1921.4	4.14	126.93	122.79
20	2738.5	1532.4	4.34	126.22	121.98
Notes：T_g1 is the SEBS glass transition temperature, T_g2 is the PPS glass transition temperature, and ΔT_g is the discrepancy between glass transition temperatures.

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表 2 不同SEBS含量的SEBS/PPS复合材料DSC热力学参数

Table 2. DSC thermodynamic parameters of SEBS/PPS composites with different SEBS contents

Content of SEBS /wt%	T_c/℃	T_m/℃	$\Delta {H_m}$/(J·g⁻¹)	X_c/%
0	236.4	285.3	37.670	34.1
3	236.3	285.2	36.420	34.0
6	235.7	285.0	34.871	33.6
9	235.1	284.8	32.435	33.4
15	234.6	284.5	30.463	33.3
20	233.8	283.2	22.597	28.3
Notes：T_c is the crystallization temperature, T_m is the melting temperature, ΔH_m is the enthalpy of melting, and X_c is the degree of crystallinity, calculated according to equation (1).

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