Influence of Nucleation-growth Liquid-liquid Phase Partition on Properties of Lead-free Low Temperature Frit

doi:10.11901/1005.3093.2021.005

Chinese Journal of Materials Research

2021, Vol. 35

Issue (9): 657-666 DOI: 10.11901/1005.3093.2021.005

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Influence of Nucleation-growth Liquid-liquid Phase Partition on Properties of Lead-free Low Temperature Frit

WANG Peng¹, LU Xilong¹^,²(

), CAO Chun-e¹(

), CHEN Yunxia¹^,², SHEN Huarong¹, ZHANG Xu¹

^1.College of Materials Science and Engineering, Jingdezhen Ceramic Institute, Jingdezhen 333403, China
^2.Jingdezhen Key Laboratory of Environmental Ceramic Materials, Jingdezhen 333000, China

Cite this article:

WANG Peng, LU Xilong, CAO Chun-e, CHEN Yunxia, SHEN Huarong, ZHANG Xu. Influence of Nucleation-growth Liquid-liquid Phase Partition on Properties of Lead-free Low Temperature Frit. Chinese Journal of Materials Research, 2021, 35(9): 657-666.

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Abstract

The nucleation-growth type liquid-liquid nano-phase partitioned low-temperature frits were prepared via a two-step process: high-temperature melting and low-temperature heat treatment. The influence of the phase-partition on the gloss, gloss loss, microhardness and other properties of the ABS* lead-free low-temperature frit were assessed by means of high temperature microscopy, differential scanning calorimetry, X-ray diffractometer, scanning electron microscopy, transmission electron microscopy and Fourier transform infrared spectroscopy. The results show that the size, volume fraction and distribution of the dispersed phase can be effectively adjusted with the aid of appropriate heat treatment processes. The heat-treated frits present microhardness and wear resistance much higher than those of the water-quenched ones. With the increasing heat treatment temperature, the gloss loss of the frits experienced a "Z" shaped variation and the microhardness experienced a reverse trend. Being heat treated at 630℃, the frit presents the smallest gloss loss of 26.4%, the largest hardness of 6202 MPa, whilst its wear resistance can be classified as grade 2 (750 revolutions). The size and the volume of the phase-partition generated dispersive droplets show a downward parabola-like variation as the heat treatment temperature increases. The phase partition facilitates the enrichment of alkali, cerium and boron in the dispersed phase. As the size and volume fraction of the dispersed phases in the frit increases, the free oxygen in the continuous matrix decreases, that is, the O/Si ratio decreases, while the amount of [SiO₄] and bridge oxygen increases and the polymerization degree of the network increases. Besides the frit has a dense surface layer, namely the phase-partitioning structure exists inside the frit. The phase rich in alkali, cerium and boron dispersed and embedded in the Si-rich continuous matrix as droplets, in other words the former is protected by the later one. Therefore, the wear resistance and microhardness of the frits were enhanced .

Key words: inorganic non-metallic materials glass and amorphous low-temperature frit heat treatment phase separation alkali borosilicate

Received: 13 January 2021

ZTFLH:

TQ174.4

Fund: National Natural Science Foundation of China(51862019);Foundation of Jiangxi Provincial Department of Education(GJJ160883);Science and Technology Project of Jingdezhen(20182GYDZ011-16)

About author: CAO Chun-e, Tel: 13707983241, E-mail: tycce@163.com
LU Xilong, Tel: 13979831378, E-mail: luxilong@jci.edu.cn

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	Peng WANG
	Xilong LU
	Chun-e CAO
	Yunxia CHEN
	Huarong SHEN
	Xu ZHANG

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https://www.cjmr.org/EN/10.11901/1005.3093.2021.005 OR https://www.cjmr.org/EN/Y2021/V35/I9/657

Table 1 Chemical composition of baseline frit R0 (mol fraction, %)

Table 2 Non-isothermal heat treatment system for frit R0

Fig.1 DSC curve of frit R0

Fig.2 XRD patterns of some samples

Fig.3 High-temperature microscope photo of frit R0

Fig.4 The area of front projected test piece silhouettes vs temperature

Table 3 The effect of non-isothermal heat treatment on the performance of frits

Fig.5 Gloss loss vs final treatment temperatures

Fig.6 Vickers hardness vs different final treatment temperatures

Fig.7 SEM cross-section images of frit samples R0 (a), R1 (b), R3 (c) and R4 (d)

Fig.8 Frit phase separation droplet size distribution R0 (a), R1 (b), R3 (c) and R4 (d)

Fig.9 Volume fraction and average size of phase-separated droplets in frit

Fig.10 TEM photo of sample R0

Fig.11 TEM photo of sample R3

Fig.12 TEM images and EDS spectra of sample R3

Table 4 The composition of three points A, B, C in the TEM image of R3

Fig.13 SEM cross-section images of sample R3

Fig.14 FTIR spectra of samples

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