首页|Pd/CeO2上乙酸丁酯高效深度氧化性能与机理研究

Pd/CeO2上乙酸丁酯高效深度氧化性能与机理研究

扫码查看
新能源汽车和相关领域中,对于典型含氧挥发性有机物乙酸丁酯的治理越来越重要.通过引入0.5%的Pd来调节CeO2-U催化剂的表面结构和理化性质,并与含等量Pd的Al2O3和TiO2进行对比,通过SEM、XPS、in-situ DRIFTS等手段对催化剂进行表征,以探究Pd和Ce活性组分间的协同作用对乙酸丁酯(BA)催化氧化性能的影响.研究结果表明,在220 ℃下引入Pd使CeO2-U的CO2产率由77.8%提高至90.7%,明显促进了 BA的深度氧化进程,缓解了CO2选择性滞后的问题.Pd的引入改善了 CeO2中晶格氧的移动性和反应性,增加了表面Ce3+的含量,提高了表面氧空位浓度.结合in-situ DRIFTS图谱分析,证实了 Pd/CeO2-U上BA的催化氧化机理,即在低温段(T<200 ℃)遵循 Langmuir-Hinshelwood(L-H)机理,在高温段(T>200℃)遵循 Mars-van Krevelen(MvK)反应机理,并且发现中间产物羧酸盐的分解为关键的控速步骤.本研究结果可为相关领域乙酸丁酯的治理提供借鉴.
Study on the performance and mechanism of high-efficiency deep oxidation of butyl acetate over Pd/CeO2
In the field of new energy vehicles and related sectors,treating butyl acetate(BA),a typi-cal oxygen-containing volatile organic compound(VOC),is becoming increasingly important.The sur-face structure and physicochemical properties of a CeO2-U catalyst were adjusted by introducing 0.5%Pd,and compared with Al2O3 and TiO2 catalysts containing the same Pd loading.Characterizations using SEM,XPS,in-situ DRIFTS,and other methods were conducted to explore the synergistic effect of Pd and Ce active components on catalytic oxidation of BA.The results showed that the introduction of Pd increased CeO2-U's CO2 yield from 77.8%to 90.7%at 220 ℃,significantly promoting the deep oxidation process of BA and alleviating the issue of CO2 selectivity delay.The introduction of Pd en-hanced the mobility and reactivity of lattice oxygen in CeO2,increased the proportion of surface Ce3+,and boosted surface oxygen vacancy concentration.Additionally,the catalytic oxidation mechanism of BA over Pd/CeO2-U was confirmed through in-situ DRIFTS analysis,indicating that the L-H mecha-nism was followed at low temperatures(T<200 ℃),while the MvK reaction mechanism occurred fol-lowed at high temperatures(T>200 ℃).It was found that the decomposition of intermediate carbox-ylate served as the rate-controlling step.These findings have implications for controlling BA in the field of related sectors.

Butyl acetatePd/CeO2Catalytic oxidationCO2 selectivityOxygen vacancy

孔文晶、林佳佳、钟雪芸、邢赟、刘鹏、李振国、付名利

展开 >

华南理工大学环境与能源学院,广东广州 510006

广东省大气环境与污染控制重点实验室,广东广州 510006

中国汽车技术研究中心有限公司移动源排放控制技术国家工程实验室,天津 300300

乙酸丁酯 Pd/CeO2 催化氧化 CO2选择性 氧空位

国家移动源排放控制技术工程实验室国家自然科学基金面上资助项目

NELMS2020A0651878293

2024

能源环境保护
煤炭科学研究总院杭州环境保护研究所

能源环境保护

影响因子:0.472
ISSN:1006-8759
年,卷(期):2024.38(4)
  • 9