Enhanced low temperature catalytic activity for toluene oxidation over core-shell LaMnO3@α-MnO2 catalyst with oxygen vacancies

Enhanced low temperature catalytic activity for toluene oxidation over core-shell LaMnO3@α-MnO2 catalyst with oxygen vacancies
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氧空位核壳LaMnO3@α-MnO2催化剂增强甲苯氧化低温催化活性

DOI:
10.1016/j.chphi.2022.100117
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发表时间:
2022-10
影响因子:
2.2
通讯作者:
Haibao Huang
Haibao Huang
中科院分区:
--
文献类型:
--
作者:
Jing Huang;Ruimei Fang;Xinyue Huang;Xiao'ai Luo;Yanjuan Sun;Fan Dong;Haibao Huang

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在MnO 2基复合氧化物催化剂上引入氧空位是提高催化剂在多相反应(如挥发性有机物(VOCs)氧化反应)中活性的有效途径。采用水热法制备了核壳结构LaMnO3@α-MnO 2催化剂,并将其用于甲苯氧化反应。不规则核壳结构的L@M-10催化剂表现出优异的低温催化活性和稳定性,在200 °C时达到100%的甲苯去除率。即使在五个重复循环之后,起燃温度(T50)和完全转化温度(T90)也分别为235 ° C和271 °C。L@M-10样品的界面效应促进了氧空位的产生,有利于活性氧物种的形成。结合原位DRIFTS结果,提出了甲苯在L@M-10催化剂上氧化反应的可能机理。L@M-10样品的开环反应速度快,羧酸或酸酐快速转化为CO2和H2O,说明其具有上级的催化性能和稳定性。本工作重点研究了界面效应对LaMnO3@α-MnO 2催化剂甲苯氧化活性和稳定性的影响,为界面效应在热催化反应中的应用提供了新的思路。
Engineering oxygen vacancies is an effective strategy to enhance the catalytic activity of MnO2based composite oxides in heterogenous reactions, such as volatile organic compounds (VOCs) oxidation reaction. Core-shell structure LaMnO3@α-MnO2catalysts were prepared by hydrothermal method via varying the concentrations of LaMnO3and used in toluene oxidation reaction. Irregular core-shell structure L@M-10 catalyst exhibits excellent low temperature catalytic activity and stability, achieving 100% toluene removal efficiency at 200 °C. The light-off temperature (T50) and complete conversion temperature (T90) are 235 and 271 °C even after five repetitive cycles, respectively. The interfacial effect of L@M-10 sample promotes the generation of oxygen vacancies, facilitating the formation of active oxygen species. A possible oxidation reaction mechanism of toluene over L@M-10 catalyst was proposed in combination with thein-situDRIFTS results. Fast ring-opening reaction and quick transformation of carboxylate or anhydride species into final products CO2and H2O explains the superior catalytic property and stability of L@M-10 sample. This work highlights the effect of interface on the catalytic activity and stability of LaMnO3@α-MnO2catalyst towards toluene oxidation and can offer a new insight into the utilization of interfacial effect in thermocatalytic reactions.
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