College of Environment and Energy, South China University of Technology
Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control
National Engineering Laboratory for Mobile Source Emission Control Technology, ChinaAutomotive Technology & Research Center Co., Ltd.

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-situDRIFTS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-situDRIFTS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-vanKrevelen(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。

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 CeO-U catalyst were adjusted by introducing 0.5%Pd, and compared with AlO and TiO catalysts containing the same Pd loading. Characterizationsusing SEM, XPS, in-situ DRIFTS, and other methods were conducted to explore the synergistic effectof Pd and Ce active components on catalytic oxidation of BA. The results showed that the introduction ofPd increased CeO-U′s CO yield from 77.8% to 90.7% at 220 ℃, significantly promoting the deepoxidation process of BA and alleviating the issue of CO selectivity delay. The introduction of Pd en⁃hanced the mobility and reactivity of lattice oxygen in CeO, increased the proportion of surface Ce,and boosted surface oxygen vacancy concentration. Additionally, the catalytic oxidation mechanism ofBA over Pd / CeO-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 fieldof related sectors.

国家移动源排放控制技术工程实验室(NELMS2020A06);国家自然科学基金面上资助项目(51878293)

孔文晶,林佳佳,钟雪芸,等.Pd/CeO2上乙酸丁酯高效深度氧化性能与机理研究[J].能源环境保护,2024,38(4):198-208.

KONG Wenjing, LIN Jiajia, ZHONG Xueyun, et al. Study on the performance and mechanism of high-efficiencydeep oxidation of butyl acetate over Pd/ CeO2[J]. Energy Environmental Protection, 2024, 38(4): 198-208.