无机材料学报 ›› 2024, Vol. 39 ›› Issue (6): 681-690.DOI: 10.15541/jim20230546
收稿日期:
2023-11-29
修回日期:
2023-12-29
出版日期:
2024-06-20
网络出版日期:
2024-01-08
通讯作者:
孙佳, 副教授. E-mail: j.sun@nwpu.edu.cn;作者简介:
张育育(1997-), 女, 博士研究生. E-mail: Zhangyuyu@mail.nwpu.edu.cn
基金资助:
ZHANG Yuyu(), WU Yicheng, SUN Jia(
), FU Qiangang(
)
Received:
2023-11-29
Revised:
2023-12-29
Published:
2024-06-20
Online:
2024-01-08
Contact:
SUN Jia, associate professor. E-mail: j.sun@nwpu.edu.cn;About author:
ZHANG Yuyu (1997-), female, PhD candidate. E-mail: Zhangyuyu@mail.nwpu.edu.cn
Supported by:
摘要:
聚合物转化SiCN陶瓷得益于质量轻和热膨胀系数低等优势, 在电磁波吸收领域受到广泛关注。由于电磁损耗机制单一及耐温性不足, SiCN陶瓷的吸波性能有待进一步提高, 借助多组元协同作用增强吸波性能是可行的途径之一。本工作对聚氮硅烷结合不同化合物进行单源化改性得到SiHfCN、SiHfCN-C、SiHfCN-B和SiHfCN-N等四种纳米陶瓷。结果表明:SiHfCN中由于Hf源的含氧量高达13.5%(质量分数), 生成HfO2和SiO2, 使其最低反射损耗(Reflection loss, RLmin)仅为-13.8 dB, 有效吸收带宽(Effective absorption bandwidth, EAB)仅为0.42 GHz。相比于SiHfCN, 含Hf聚合物分别与C源、B源和N源共改性增加了聚合物转化陶瓷的界面和导电相, SiHfCN-C、SiHfCN-B和SiHfCN-N的介电常数实部和虚部分别提高了1.4~1.8和2.7~3.9倍, RLmin分别为-50.6、-57.3和-63.5 dB, EAB分别为3.53、3.99和4.01 GHz, 吸波性能得到了显著改善。SiHfCN-C中大量的自由碳抑制了HfO2的生成, 增强了电导损耗。SiHfCN-B中生成了B-N和B-C键, 且析出的纳米棒状HfSiO4提供了更多的异质界面, 增强了极化损耗。SiHfCN-N中因引入大量N使N-C键数量增加, 强化了偶极子极化损耗, 同时生成纳米碳片, 不仅可以增强电导损耗, 而且提供大量界面, 改善了阻抗匹配并增强了界面极化, 因而SiHfCN-N具有最佳的吸波性能。
中图分类号:
张育育, 吴轶城, 孙佳, 付前刚. 聚合物转化SiHfCN陶瓷的制备及其吸波性能[J]. 无机材料学报, 2024, 39(6): 681-690.
ZHANG Yuyu, WU Yicheng, SUN Jia, FU Qiangang. Preparation and Wave-absorbing Properties of Polymer-derived SiHfCN Ceramics[J]. Journal of Inorganic Materials, 2024, 39(6): 681-690.
SSPs | PDCs | PSN | Hf isopropoxide isopropanol complex | DVB | Melamine | Dimethylamino borane |
---|---|---|---|---|---|---|
P7Hf3 | SiHfCN | 7 | 3 | - | - | - |
P7Hf3-C | SiHfCN-C | 7 | 3 | 6 | - | - |
P7Hf3-N | SiHfCN-N | 7 | 3 | - | 6 | - |
P7Hf3-B | SiHfCN-B | 7 | 3 | - | - | 6 |
表1 不同样品的原料比例(%, 质量分数)
Table 1 Raw material proportions (%, in mass) of different samples
SSPs | PDCs | PSN | Hf isopropoxide isopropanol complex | DVB | Melamine | Dimethylamino borane |
---|---|---|---|---|---|---|
P7Hf3 | SiHfCN | 7 | 3 | - | - | - |
P7Hf3-C | SiHfCN-C | 7 | 3 | 6 | - | - |
P7Hf3-N | SiHfCN-N | 7 | 3 | - | 6 | - |
P7Hf3-B | SiHfCN-B | 7 | 3 | - | - | 6 |
Element | SiHfCN | SiHfCN-C | SiHfCN-N | SiHfCN-B |
---|---|---|---|---|
Si | 35.5 | 42.3 | 40.8 | 33.8 |
Hf | 22.5 | 18.6 | 20.4 | 13.5 |
C | 13.6 | 24 | 8.2 | 13.3 |
N | 22.8 | 9.4 | 55.5 | 29.8 |
O | 5.6 | 5.7 | 7.1 | 5.3 |
Empirical formula | SiHf0.10C0.90N1.29O0.28 | SiHf0.07C1.33N0.45O0.24 | SiHf0.08C0.47N2.73O0.31 | SiHf0.06C0.92N1.77O0.28B0.33 |
表2 PDCs的元素含量(%, 质量分数)和经验化学式
Table 2 Elemental contents (%, in mass) and empirical chemical compositions of the PDCs
Element | SiHfCN | SiHfCN-C | SiHfCN-N | SiHfCN-B |
---|---|---|---|---|
Si | 35.5 | 42.3 | 40.8 | 33.8 |
Hf | 22.5 | 18.6 | 20.4 | 13.5 |
C | 13.6 | 24 | 8.2 | 13.3 |
N | 22.8 | 9.4 | 55.5 | 29.8 |
O | 5.6 | 5.7 | 7.1 | 5.3 |
Empirical formula | SiHf0.10C0.90N1.29O0.28 | SiHf0.07C1.33N0.45O0.24 | SiHf0.08C0.47N2.73O0.31 | SiHf0.06C0.92N1.77O0.28B0.33 |
图5 PDCs的SEM照片及EDS分析
Fig. 5 SEM images and EDS analyses of the PDCs (a) SiHfCN; (b) SiHfCN-C; (c) SiHfCN-N; (d) SiHfCN-B; (e) Elemental contents (%, in atom) of spots in (a-d)
图6 SiHfCN和SiHfCN-C的TEM照片
Fig. 6 TEM images of SiHfCN and SiHfCN-C (a-d) SiHfCN; (e-h) SiHfCN-C; (a, e) Bright field images; (b, c, f, g) HRTEM images with corresponding SAED inserted; (d, h) EDS mappings
图7 SiHfCN-N和SiHfCN-B的TEM照片
Fig. 7 TEM images of SiHfCN-N and SiHfCN-B (a-d) SiHfCN-N; (e-h) SiHfCN-B; (a, e) Bright field images; (b, c, f, g) HRTEM images with corresponding SAED inserted; (d, h) EDS mappings
图8 PDCs的电磁参数
Fig. 8 Electromagnetic parameters of the PDCs (a) Real part; (b) Imaginary part; (c) Loss tangent; (d) Attenuation coefficient; (e, f) Cole-Cole curves; Colorful figures are available on website
图9 PDCs的RL图和阻抗匹配图
Fig. 9 RL patterns and impedance matching maps of the PDCs (a-h) RL patterns; (i-l) Impedance matching maps; (a, b, i) SiHfCN; (c, d, j) SiHfCN-C; (e, f, k) SiHfCN-N; (g, h, l) SiHfCN-B
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