Co3O4改性USY分子筛吸附和催化氧化甲苯特性研究

doi:10.11949/0438-1157.20201735

摘要/Abstract

摘要：

利用水热法合成Co₃O₄/USY复合材料，研究其对有机污染物甲苯的吸附和催化氧化特性，同时结合微波对Co₃O₄的精准加热特性，考察不同负载量Co₃O₄/USY在微波作用下的升温特性及催化甲苯氧化降解特性。结果表明，通过水热反应，Co₃O₄在USY表面形成多孔蜂窝状结构；负载Co₃O₄后的USY保持较高的吸附容量，Co₃O₄/USY-1.5m室温下的吸附容量为85 mg/g；Co₃O₄/USY在干、湿两种状态下均在325℃表现出优良的催化氧化特性、CO₂选择性和稳定性；Co₃O₄/USY能够与微波高效耦合，快速升温启动其催化作用，控制反应温度为250℃，发现微波诱导甲苯催化氧化过程的CO₂选择性优于常规催化，表明所制备Co₃O₄/USY复合材料具备吸附甲苯并进行微波快速再生协同有机污染物高效催化氧化降解的可行性。

关键词: Co₃O₄/USY, 复合材料, 分子筛, 吸附, 催化氧化, 微波, VOCs

Abstract:

Co₃O₄/USY composite material was synthesized by a hydrothermal method. Experimental study was conducted to investigate its absorption and catalytic oxidation characteristics of organic pollutant toluene. Since the Co₃O₄ can be efficiently heated by microwaves, the heating characteristics and catalytic oxidation of toluene on Co₃O₄ modified USY under microwave action were also investigated, with an aim to discuss the feasibility of microwave-assisted rapid regeneration of adsorbent whilst in-situ degradation of organic matter. By hydrothermal reaction, Co₃O₄ forms a porous cellular structure on the surface of USY. The USY loaded with Co₃O₄ maintains high adsorption capacity, and the adsorption capacity of Co₃O₄/USY-1.5m at room temperature is 85 mg/g. The prepared Co₃O₄/USY composite material exhibits excellent catalytic oxidation properties, CO₂ selectivity and stability at 325℃ in both dry and wet conditions. The prepared Co₃O₄/USY composite material can couple with microwave in an efficient way, leading to quick start up its catalytic function. Comparative study shows that the CO₂ selectivity and catalysis stability under the microwave heating scenario are better than conventional heating when the reaction temperature is controlled at 250℃. The above results indicate that the prepared Co₃O₄/USY composite material can be used as an adsorbent to adsorb toluene and regenerated by microwave heating whilst the desorbed organic matter can be efficiently degraded by in situ catalytic oxidation.

Key words: Co₃O₄/USY, composite material, molecular sieve, adsorption, catalytic oxidation, microwave, VOCs

中图分类号:

TQ 028.8

孙静, 董一霖, 李法齐, 李文翔, 马晓玲, 王文龙. Co₃O₄改性USY分子筛吸附和催化氧化甲苯特性研究[J]. 化工学报, 2021, 72(6): 3306-3315.

SUN Jing, DONG Yilin, LI Faqi, LI Wenxiang, MA Xiaoling, WANG Wenlong. Study on adsorption and catalytic oxidation characteristics of toluene on Co₃O₄ modified USY molecular sieve[J]. CIESC Journal, 2021, 72(6): 3306-3315.

图/表 10

图1 吸附/催化实验系统示意图

Fig.1 Schematic diagram of adsorption / catalysis experimental system

图2 Co3O4/USY吸附剂XRD谱图

Fig.2 XRD patterns of Co3O4/USY adsorbent

图3 USY(a)、Co3O4/USY-1.5m(b)、Co3O4/USY-2m(c)及Co3O4/USY-3m(d)的SEM图

Fig.3 SEM images of USY (a), Co3O4/USY-1.5m (b), Co3O4/USY-2m (c) and Co3O4/USY-3m(d)

表1 USY和Co3O4/USY复合材料的BET分析

Table 1 BET analysis of USY and Co3O4/USY composite materials

材料	总比表面积/(m²/g)	微孔表面积/(m²/g)	外表面积/(m²/g)	总孔容/(cm³/g)	微孔孔容/(cm³/g)	介孔孔容/(cm³/g)	平均孔径/nm
USY	828	732	96	0.44	0.28	0.16	1.36
Co₃O₄/USY-1.5m	584	359	226	0.56	0.17	0.39	2.27
Co₃O₄/USY-2m	524	260	264	0.62	0.11	0.51	2.64
Co₃O₄/USY-3m	449	265	184	0.54	0.11	0.43	2.76

图4 USY及Co3O4/USY复合材料对甲苯的吸附性能

Fig.4 Curves of toluene adsorption by USY and Co3O4/USY composite materials

图5 Co3O4/USY催化甲苯氧化特性

Fig.5 Catalytic performance of Co3O4/USY for toluene oxidation

图6 Co3O4/USY在干、湿条件下催化甲苯氧化特性

Fig.6 Catalytic performance of Co3O4/USY for toluene oxidation under dry and wet conditions

图7 Co3O4/USY-1.5m在干态(a)及不同湿度(b)条件下催化甲苯稳定性

Fig.7 Co3O4/USY-1.5m catalytic stability for toluene oxidation under dry state (a) and different humidity conditions(b)

图8 Co3O4/USY在微波作用下的升温特性

Fig.8 Heating characteristics of Co3O4/USY under microwave action

图9 常规加热(a)和微波加热(b)250℃条件下催化甲苯的对比特性(N表示常规催化；M表示微波催化)

Fig.9 Comparison of catalytic toluene under conventional heating (a) and microwave heating conditions (b) at 250℃

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Co₃O₄改性USY分子筛吸附和催化氧化甲苯特性研究

Study on adsorption and catalytic oxidation characteristics of toluene on Co₃O₄ modified USY molecular sieve

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