ISSN 1008-5548

CN 37-1316/TU

2024年30卷  第3期
<返回第3期

陶瓷蜂窝净化材料的制备及吸附性能

Preparation of honeycomb ceramics purification materials and their adsorption performance


付 琳1 ,姬文晋1 ,何家俊1 ,黄超强1 ,李永峰1,2 ,窦永深2

(1. 广东工业大学 轻工化工学院,广东 广州 510006;2. 佛山市顺德区金磊环保科技有限公司,广东 佛山 528308)


引用格式:

付琳,姬文晋,何家俊,等. 陶瓷蜂窝净化材料的制备及吸附性能[J]. 中国粉体技术,2024,30(3):170-182.

FU L, JI W J, HE J J,et al. Preparation of honeycomb ceramics purification materials and their adsorption performance[J].China Powder Science and Technology,2024,30(3):170−182.

DOI:10.13732/j.issn.1008-5548.2024.03.015

收稿日期:2023-11-15,修回日期:2023-12-18,上线日期:2024-04-16。

基金项目:国家自然科学基金项目,编号:22278086。

第一作者简介:付琳(2000—),女,硕士生,研究方向为有机污染物净化治理。E-mail:1639545624@qq. com。

通信作者简介:李永峰(1976— ),男,教授,博士,广州市珠江科技新星,硕士生导师,研究方向为大气污染物净化治理。E-mail:gdliyf@gdut. edu. cn。


摘要:【目的】 为了去除三甲胺异味污染物,分析不同改性方法对陶瓷蜂窝吸附净化三甲胺性能的影响。【方法】 采用涂覆工艺,在陶瓷蜂窝基底上负载金属离子活性涂层制备整体式净化材料,以三甲胺的吸附容量作为净化评价指标,研究涂覆工艺参数优化和金属离子改性规律。【结果】 陶瓷蜂窝净化材料的最优制备工艺条件为:胶黏剂类型为铝溶胶,添加的尿素浓度为0. 9 mol/L,热处理温度为120~150℃,添加的金属离子为Ca2+ 和Fe3+ 、浓度为0. 3 mol/L。用Ca2+ 离子改性的陶瓷蜂窝净化材料三甲胺饱和吸附容量可达到368 mg/g,且在多次热再生后重复使用时净化性能保持不变;制备规模放大10倍后,所制得的陶瓷蜂窝材料也能保持三甲胺吸附净化性能。【结论】 金属离子改性陶瓷蜂窝净化材料可有效去除三甲胺等异味污染物,具有饱和吸附量高、可多次重复使用等特点;净化材料制备规模放大后的净化性能保持重现性,具备规模化生产潜质。

关键词:净化材料;三甲胺;陶瓷蜂窝;涂覆工艺

Abstract

Objective Trimethylamine, a toxic, nitrogen-containing volatile organic compound, is widely recognized as an indoor odor pollutant, with its pungent odor significantly contributing to external air pollution. Microbiota can easily metabolize trimethylamine pollutants, leading to the formation of trimethylamine-n-oxide, which is closely linked to various cardiovascular diseases. Therefore, there is an urgent need to purify such odor pollutants for people's well-being. In this paper, the effects of different modification methods on the adsorption and purification performance of ceramic honeycomb purification materials for trimethylamine was thoroughly analyzed, ultimately aiming to achieve efficient purification of trimethylamine odor pollutants.

Methods A coating technology was used to directly apply metal ion active coatings onto ceramic honeycomb substrates, forming integrated chemical purification materials. The process involved several steps: Firstly, the ceramic honeycomb substrate underwent pretreatment, including pickling, ultrasonic treatment, and high temperature calcination. Secondly, the pre-treated substrate was immersed into the mixed coating slurry containing aluminum sol, urea and metal ion salt for 10 h. Finally, the coating sample was extracted, residual slurry was purged, and then the sample was dried within a temperature range of 100 to 200 ℃ for 10 h to obtain the monolithic ceramic honeycomb purification material modified with different metal ions. The static adsorption capacity of trimethylamine was employed as the evaluation index for the purification efficiency of odor pollutants. The optimization of coating process parameters, including adhesive type, concentration of added urea, thermal treatment temperature, and the modification of metal ions, was comprehensively examined, taking ino account different types and concentrations of metal ions.

Results and Discussion The adsorption capability of the pure ceramic honeycomb substrate for trimethylamine was not promi nent. However, upon modification with different adhesives, the trimethylamine adsorption capacity curve revealed that materials modified with aluminum sol exhibited the highest adsorption performance, followed by silica sol and water. The adsorption performance of the modified ceramic honeycomb material for trimethylamine improved with increasing concentration of the poremaking agent urea. However, at a urea concentration of 1. 2 mol/L, there was no significant improvement in the adsorption capacity of the modified ceramic honeycomb material for trimethylamine. Additionally, the adsorption capacity of trimethylamine on ceramic honeycomb materials initially increased and then declined with the increase of heat treatment temperature. At a heat treatment temperature from 120 to 150 ℃, the ceramic honeycomb material exhibited optimaladsorption performance for trimethylamine. The sequence of adsorption capacities for different metal ions, ranked from highest to lowest, was Ca2+, Fe3+, Zn2+, Cu2+ and Mg2+, respectively. The adsorption capacities of modified Ca2+ and Fe3+ ceramic honeycomb materials for trimethylamine were 368 mg/g and 341 mg/g, respectively. As the concentration of metal ions increased, the adsorption capacity of ceramic honeycomb material for trimethylamine initially rose and then declined. When the concentration of metal ions was 0.3 mol/L,the modified ceramic honeycomb material exhibited optimal adsorption performance for trimethylamine. In summary, the optimum preparation conditions for ceramic honeycomb purification materials can be determined as follows:choosing aluminum sol as the adhesive, setting the concentration of urea additive at 0.9 mol/L,selecting a heat treatment temperature between 120 and 150 ℃, using Ca2+ and Fe3+ as metal ion additives, and maintaining a concentration of metal ion additive at 0. 3 mol/L.

Compared to pure ceramic honeycomb materials,metal-ion-modified ceramic honeycomb purification materials, coated with aluminum sol and urea additive, exhibited a significan enhancement in the adsorption capacity of trimethylamine. The adsorption capacity of trimethylamine could increase by hundreds of times compared to the unmodified material. Furthermore, even after thermal regeneration and repeated use of the same purification material, the decrease in trimethylamine adsorption performance was minimal. Additionally, upon scaling up the preparation by tenfold, the static adsorption capacity of the entire chemical purification material, obtained by the same preparation process for trimethylamine pollutants, remained consistent with that of the small-scale purification material. Overall, the saturation adsorption capacity of Ca2+ modified ceramic honeycomb material for trimethylamine reached 368 mg/g. Even after repeated thermal regeneration, the purification performance of ceramic honeycomb material for trimethylamine remained unchanged. Simultaneously, the ceramic honeycomb material obtained after a tenfold enlargement of a single batch could still maintain the adsorption and purification properties of trimethylamine. These results indicate that the preparation method is simple, the adsorption properties are commendable, and the obtained ceramic honeycomb purification material has significant potential for largescale production.

Conclusion The as-prepared ceramic honeycomb purification material modified by metal ions proves to behighly effective in removing odor pollutants such as trimethylamine. Itboaststhe advantages such as high saturated adsorption capacity and the ability for repeated use. Moreover,the ceramic honeycomb material has good amplification repeatability and has the potential of large-scale production,allowing it well-suited for widespread application in the field of odor air purification.

Keywords:purification material;trimethylamine;ceramic honeycomb;coating process


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