高温除尘碳化硅膜的制备及其抗腐蚀特性

doi:10.11949/j.issn.0438-1157.20180960

摘要/Abstract

摘要：

采用喷涂法在碳化硅（SiC）支撑体上覆膜，根据碳化硅材料的氧化特性，设计了有氧烧结和氩气烧结随温度转换的组合烧结制度，并通过优化保温时间降低碳化硅陶瓷膜烧结成本。研究结果表明，新的烧结制度能有效地控制有氧烧结阶段产生的二氧化硅（SiO₂）量，并促进其与烧结助剂氧化锆（ZrO₂）等在气氛烧结阶段的反应，反应生成的锆英石相和添加莫来石相共同形成SiC颗粒连接颈部。制备的碳化硅陶瓷膜平均孔径为3.03 μm，气体通量为175 m³?m^-2?h^-1?kPa^-1。且在100℃的0.25 mol?L^-1的H₂SO₄溶液和0.25 mol?L^-1的NaOH溶液中腐蚀6 h后，膜层表面形貌无明显变化，具有较强的抗腐蚀性能。

关键词: 除尘, 碳化硅陶瓷膜, 气氛烧结, 保温时间, 耐腐蚀

Abstract:

Spray-coating was used to prepared silicon carbide (SiC) membranes on the surface of SiC supports, then the coated samples were sintered by switching sintering atmospheres (aerobic to argon) over different temperature ranges according to the oxidation characteristics of SiC, and the sintering cost of SiC ceramic membranes was reduced by optimizing the soaking time. The results revealed that the new sintering procedures can effectively control the oxidation of SiC in the aerobic sintering stage, and promoted its oxidation product silica （SiO₂） reaction with the sintering aids such as zirconia (ZrO₂) in the argon sintering stage. The average pore size of the prepared SiC ceramic membrane was 3.03 μm and the gas permeation was 175 m³·m^-2·h^-1·kPa^-1. After etching for 6 h in 0.25 mol·L^-1 H₂SO₄ solution and 0.25 mol·L^-1 NaOH solution at 100℃, the surface morphology of the film has no obvious change and has strong corrosion resistance.

Key words: dust removal, SiC ceramic membrane, atmosphere sintering, soaking time, corrosion resistant

中图分类号:

TQ 174.6

李冬燕, 魏巍, 韩峰. 高温除尘碳化硅膜的制备及其抗腐蚀特性[J]. 化工学报, 2019, 70(1): 336-344.

Dongyan LI, Wei WEI, Feng HAN. Preparation and corrosion resistance of SiC membrane using for dust removal in high temperature[J]. CIESC Journal, 2019, 70(1): 336-344.

图/表 17

图1 碳化硅支撑体表面电镜照片

Fig.1 SEM image of surface of SiC supports

图2 碳化硅支撑体孔径分布

Fig.2 Pore size distribution of SiC membranes

图3 涂膜液的制备工艺

Fig.3 Schematic diagram of preparation of coating solution

图4 原料粉体的粒径分布

Fig.4 Particle size distribution diagram of raw materials

图5 碳化硅粉体的热重分析

Fig.5 TGA of α-SiC powder

图6 碳化硅陶瓷膜生坯氧化后表面形貌变化图

Fig.6 SEM image of surface of SiC membrane after oxidation

图7 碳化硅陶瓷膜烧结制度

Fig.7 Sintering procedure of SiC membrane

图8 碳化硅膜表面形貌随有氧烧结阶段保温时间的变化

Fig.8 Effect of soaking time in aerobic sintering stage on SEM micrograph of SiC membranes

图9 碳化硅陶瓷膜XRD随有氧烧结阶段保温时间的变化

Fig.9 Effect of soaking time in aerobic sintering stage on XRD of SiC membranes

图10 碳化硅陶瓷膜孔径分布随有氧烧结阶段保温时间的变化

Fig.10 Effect of soaking time in aerobic sintering stage on pore size distribution of SiC membranes

图11 碳化硅陶瓷膜气体通量随有氧烧结阶段保温时间的变化

Fig.11 Effect of soaking time in aerobic sintering stage on gas permeation of SiC membranes

图12 碳化硅膜表面形貌随气氛烧结阶段保温时间的变化

Fig.12 Effect of soaking time in argon sintering stage on SEM micrograph of SiC membranes

图13 碳化硅陶瓷膜XRD随气氛烧结阶段保温时间的变化

Fig.13 Effect of soaking time in argon sintering stage on XRD of SiC membranes

图14 碳化硅陶瓷膜平均孔径随气氛烧结阶段保温时间的变化

Fig.14 Effect of soaking time in argon sintering stage on average pore size of SiC membranes

图15 碳化硅陶瓷膜气体通量随气氛烧结阶段保温时间的变化

Fig.15 Effect of soaking time in argon sintering stage on gas permeation of SiC membranes

图16 酸碱腐蚀后碳化硅陶瓷膜的颈部形貌变化电镜图

Fig.16 SEM micrograph of combination of SiC membrane after corrosion

表1 酸碱腐蚀后碳化硅颗粒颈部全元素分析

Table 1 All elements analyzed of bridge of SiC particles after corrosion/%(atom)

Atom	Before corrosion	After acid corrosion	After alkali corrosion
C	52.43	47.45	42.89
O	8.63	7.42	6.43
Si	37.61	43.57	49.60
Al	0.71	0.75	0.49
Zr	0.21	0.11	0.18
Ca	0.41	0.70	0.41

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