Department of Chemistry and the Materials Research Center, Northwestern University, Evanston, Illinois 60208-3113, USA.
ACS Nano. 2013 Jan 22;7(1):396-407. doi: 10.1021/nn3044148. Epub 2012 Dec 24.
The high-frequency dielectric response of 0-3 polypropylene nanocomposites prepared with the activated metallocene polymerization catalyst [rac-ethylenebisindenyl]zirconium dichlororide absorbed on the native Al(2)O(3) surfaces of metallic aluminum nanoparticles is characterized. The nanocomposites produced are randomly dispersed in the polyolefin matrix with no visible defects that might degrade film dielectric properties. Electrical measurements show that as the volume fraction of Al nanoparticles is increased, the effective permittivity of the nanocomposites increases, with ε(r) values reaching ~10 at relatively low frequency (1 MHz). Because of the high permittivity and conductivity contrast between the metal nanoparticles and the polypropylene matrix, Maxwell-Wagner-Sillars theory can be applied to model the loss at high frequencies and provide insight into how the nanocomposite high frequency response scales with Al volume fraction. At higher Al nanoparticle volume fractions, mixing theories predict greater densities of nanoparticle aggregates, consistent with the experimentally observed shift of the dielectric relaxation to lower frequencies. Although these nanocomposites undergo the predicted initial dielectric relaxation with increasing frequency, the metallic nanoparticle complex permittivity imbues the higher Al volume fraction materials with relatively high, sustainable permittivities, 6, at frequencies as high as 7 GHz.
用吸附在金属铝纳米粒子的天然 Al(2)O(3)表面上的茂金属聚合催化剂 [rac-乙撑双茚基] 二氯化锆制备的 0-3 聚丙烯纳米复合材料的高频介电响应特性。所制备的纳米复合材料在聚烯烃基质中随机分散,没有可能降低薄膜介电性能的可见缺陷。电测量表明,随着 Al 纳米粒子体积分数的增加,纳米复合材料的有效介电常数增加,在相对较低的频率(1MHz)下,ε(r) 值达到约 10。由于金属纳米粒子和聚丙烯基质之间的高介电常数和电导率对比度,可以应用 Maxwell-Wagner-Sillars 理论来模拟高频损耗,并深入了解纳米复合材料高频响应如何随 Al 体积分数而变化。在更高的 Al 纳米粒子体积分数下,混合理论预测纳米粒子聚集体的密度更大,与实验观察到的介电松弛向更低频率的转移一致。尽管这些纳米复合材料随着频率的增加经历了预测的初始介电松弛,但金属纳米粒子复介电常数赋予了具有相对较高和可持续介电常数 6 的更高 Al 体积分数材料,在高达 7GHz 的频率下。