A high heat resistance, high toughness and low dielectric fluorenyl benzoxazine resin composition and its preparation method and application

Abstract

The invention discloses a high heat-resistant, high-toughness, low-dielectric fluorenyl benzoxazine resin composition and a preparation method thereof. The weight ratio is a mixture of resin: inorganic filler: accelerator: solvent = 100: 30 ~ 70: 0.01 ~ 1: 57 ~ 80; the weight ratio of resin is benzoxazine resin: DCPD epoxy resin: phosphorus phenolic Resin = 100: 40-80: 10-40 mixture; benzoxazine resin is a weight ratio of high heat resistance, high toughness, low dielectric fluorenyl benzoxazine resin: other benzoxazine resin = 60-100: A single substance or a mixture of 0 to 40; the composition of the present invention is used in the fields of laminated boards, integrated circuit packaging, high-frequency high-speed copper clad laminates and high-density Internet, and has excellent heat resistance, low dielectric constant and dielectric loss Factor, better flame retardancy and bending strength, lower water absorption, etc.

Description

technical field [0001] The invention belongs to a composition containing an organic polymer mixture and its preparation, and relates to a high heat-resistant, high-toughness, low-dielectric fluorenyl benzoxazine resin composition, its preparation method and application. The high heat-resistant, high-toughness and low-dielectric fluorenyl benzoxazine resin composition of the present invention can be used in laminated boards, integrated circuit packaging, high-frequency and high-speed copper-clad laminates, high-density Internet and other fields, and has broad application prospects. Background technique [0002] In recent years, 5G communication has become a research and development hotspot worldwide. Because of its higher reliability and faster speed, it will play a strategic leading role in China's manufacturing 2025. important basic conditions. Due to its data transmission rate and high reliability requirements, 5G communication puts forward very high requirements on the d...

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Problems solved by technology

But on the other hand, the structure of fluorenyl is too rigid, so that it will have the problems of high brittleness and low bending strength when it is applied.

In response to this problem, many patented technologies have synthesized a series of toughened and modified new fluorenyl benzoxazines through molecular design. For example, CN103936686A synthesized a tetrafunctional fluorenyl benzoxazine. By adjusting fatty amines and substituted or unsubstituted The rigid and flexible groups in the salicylaldehyde compound increase the crosslinking density of benzoxazine and improve the flexibility, but because there are four oxazine ring ring-forming positions in the molecule, the steric hindrance is relatively large, and there will be The problems of benzoxazine low cyclization rate and low product yield (45-80%), similar patents also include CN102702225A and CN103896867A

CN102634019A mentions that bisphenol compounds such as bisphenol A, bisphenol AF, bisphenol F, etc. and bisphenol fluorene are introduced into the fluorenyl benzo structure as a phenol source, and the ratio of bisphenol fluorene to bisphenol compounds is adjusted Heat resistance and flexibility, but it is difficult for this improved polymer to have both high heat resistance and high flexibility

CN102702128A and CN102702129A improve the flexibility of fluorenylbenzoxazine by introducing flexible ester groups and ether bonds, but there is also the problem of low product yield (50-85%)

Moreover, the above-mentioned patent documents only provide the molecular structure of the new fluorenylbenzo, heat resistance data (Tg: 180-390°C, Td5%: 330-420°C) and the theory of flexibility improvement, but fail to provide flexibility. Improvement effect and specific application method

And it has been verified that the dielectric properties of the fluorenylbenzoxazine castables with the above structure are poor (Dk: 3.78-4.42, Df: 0.0067-0.0098), and the high-frequency and high-speed characteristics of 5G communication require copper-clad laminates and laminates The substrate used has better dielectric properties (Dk≤3.5, Df≤0.007)

In addition, Wang Jun from Harbin Engineering University introduced a variety of alkyl segments from the amine source in the paper "Synthesis, Polymerization and Performance Research of Fluorenyl Benzoxazine", so that the synthesized alkyl fluorenyl benzoxazine The flexibility and dielectric properties are good, but because the alkyl group is connected to the amine source, the alkyl group does not remain on the main chain when the benzoxazine is cured, so the pendant alkyl group is easy to fall off, and the heat resistance of the product is poor. Poor (Tg: 180-230°C, Td5%: 310-350°C)

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