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Boosting catalytic oxidation of propane over CeO2-supported Co3O4 catalyst with strong interfacial interaction and electron transfer
Journal of Catalysis ( IF 6.5 ) Pub Date : 2024-05-01 , DOI: 10.1016/j.jcat.2024.115529
Wenjun Zhu , Yao Li , Huibin Liu , Yudi Yan , Changhai Liang

Tuning the nanoparticle-support interaction can optimize the catalytic performance of supported metal oxide catalysts for VOCs removal. Herein, a series of CoO/CeO catalysts with different strengths of interfacial interaction and electron transfer were successfully constructed via various modified wetness impregnation procedures. With the introduction of ammonium hydroxide, citric acid or H pretreatment, a stronger interfacial interaction and electron transfer were achieved due to the highly CoO dispersion and CeO surface reconstruction. The modified-synthesis CoO/CeO catalysts, particularly CoO/CeO-CA (citric acid), demonstrated superior catalytic activity (T = 296 °C, TOF = 0.337 × 10 s) and stability for propane oxidation as compared to typical wetness impregnation CoO/CeO-DI (T = 314 °C, TOF = 0.121 × 10 s). Through systematic characterizations and DFT calculation, the strong interfacial interaction and abundant reactive oxygen species facilitate the adsorption and activation of CH and O on the catalyst surface, which further promote the intermediates (carbonate/carboxyl species) transformation. These findings highlight interfacial mechanism to catalytic performance optimization of supported metal oxides.

中文翻译:


具有强界面相互作用和电子转移的 CeO2 负载 Co3O4 催化剂促进丙烷催化氧化



调节纳米颗粒-载体相互作用可以优化负载型金属氧化物催化剂去除 VOC 的催化性能。在此,通过各种改进的润湿浸渍程序成功构建了一系列具有不同界面相互作用和电子转移强度的CoO/CeO催化剂。随着氢氧化铵、柠檬酸或H预处理的引入,由于CoO的高度分散和CeO表面重构,实现了更强的界面相互作用和电子转移。与典型的湿浸渍 CoO 相比,改性合成 CoO/CeO 催化剂,特别是 CoO/CeO-CA(柠檬酸),表现出优异的催化活性(T = 296 °C,TOF = 0.337 × 10 s)和丙烷氧化稳定性。 /CeO-DI(T = 314 °C,TOF = 0.121 × 10 s)。通过系统表征和DFT计算,强烈的界面相互作用和丰富的活性氧物质促进了CH和O在催化剂表面的吸附和活化,从而进一步促进了中间体(碳酸酯/羧基物质)的转化。这些发现强调了负载金属氧化物催化性能优化的界面机制。
更新日期:2024-05-01
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