微波催化燃烧印刷包装VOCs废气的矿化途径与降解机理

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摘要结合贵金属和过渡金属催化剂的优点，采用等体积浸渍法制备了Pt-CuMnCeO_x/蜂窝纳米陶瓷整体式催化剂，考察其在微波辐照下对印刷包装VOCs（甲苯和丙酮）废气的矿化效果及催化机理.研究表明，微波功率600W，进气量5m³/h，甲苯和丙酮浓度各1000mg/m³条件下，催化剂床层温度达到300℃，双组分VOCs矿化率为82%.结合XRD和XPS表征可知，高分散的Pt颗粒与铜锰铈尖晶石活性组分在"微波热点"作用下提高了对甲苯、丙酮的低温催化效率；微波催化燃烧反应同时遵循L-H和MvK机理，不同价态金属间发生电子转移，催化剂表面产生更多的表面吸附氧和晶格氧，从而增强了VOCs分子的吸附与氧化.中间产物测试基础上，推测甲苯的氧化降解途径为甲苯→苯甲醛→苯甲酸→小分子酸→二氧化碳和水，丙酮的氧化降解途径为：丙酮→小分子醛类、酸类→二氧化碳和水.

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关键词 ： Pt, CuMnCeO_x, VOCs, 催化燃烧, 微波, 机理

Abstract：Combined with the catalytic advantages of both noble metal and transition metal catalysts, Pt-CuMnCeO_x/honeycomb nano ceramics monolithic catalyst was prepared by incipient-wetness impregnation method. The mineralization effect and catalytic mechanism of VOCs (toluene and acetone) waste gas from printing and packaging industry on the surface of Pt-CuMnCeO_x/honeycomb nano ceramics under microwave irradiation were investigated. The results showed that bed temperature reached 300℃, and the mineralization rate of two-component VOCs was 82% under conditions of microwave power 600W, airflow 5m³/h, and toluene and acetone concentrations 1000mg/m³ respectively. Based on XRD and XPS characterizations, highly dispersive Pt particles and copper, manganese, and cerium spinel active components enhanced the catalytic efficiency of toluene and acetone at low temperature in the role of microwave "hot spots". Microwave catalytic combustion reaction followed L-H mechanism and MvK mechanism simultaneously, and electron transfer occurred between different metals with different valence states resulting in more surface adsorbed oxygen and lattice oxygen formed on the catalyst surface, which promoted the adsorption and oxidation of VOCs molecules. According to intermediate products determination, it speculated that toluene was oxidized to benzaldehyde, benzoic acid, and small molecule acids gradually, and finally mineralized to carbon dioxide and water. The oxidative pathway of acetone was small molecule aldehydes and acids, and then carbon dioxide and water.

Key words： Pt CuMnCeO_x VOCs catalytic combustion microwave mechanism

收稿日期: 2021-04-26

PACS:

X511

基金资助:陕西省自然科学基金资助项目（2021JM-364）

通讯作者: 卜龙利,副教授,bolongli@xauat.edu.cn E-mail: bolongli@xauat.edu.cn

作者简介: 陈瑾(1996-),女,陕西咸阳人,西安建筑科技大学硕士研究生,主要从事大气污染控制化学方面研究.

引用本文:

陈瑾, 卜龙利, 张丹庆, 张继宾, 田野, 刘嘉栋. 微波催化燃烧印刷包装VOCs废气的矿化途径与降解机理[J]. 中国环境科学, 2021, 41(11): 5104-5113. CHEN Jin, BO Long-li, ZHANG Dan-qing, ZHANG Ji-bin, TIAN Ye, LIU Jia-dong. Mineralization and mechanism of VOCs waste gas from printing and packaging industry by microwave catalytic combustion. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(11): 5104-5113.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2021/V41/I11/5104

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