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用于高效催化丙烷完全氧化的高分散 Pd-MnO 催化剂的制备

Fabrication of highly dispersed Pd-MnO catalyst for efficient catalytic propane total oxidation.

作者信息

Feng Chao, Wang Yunxia, Chen Chong, Fu Xueqing, Pan Yuan, Xin Hongchuan, Wang Zhong, Lu Yukun, Li Xuebing, Zhang Runduo, Liu Yunqi

机构信息

State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering, China University of Petroleum, Qingdao 266580, China; Key Laboratory of Biofuels, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.

State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering, China University of Petroleum, Qingdao 266580, China.

出版信息

J Colloid Interface Sci. 2023 Nov 15;650(Pt B):1415-1423. doi: 10.1016/j.jcis.2023.07.076. Epub 2023 Jul 16.

Abstract

Adjusting the interaction between dual active components for enhancing volatile organic compounds (VOCs) degradation is an effective but still challenging means of air pollution control. Herein, a limited pyrolysis oxidation strategy was adopted to prepare Pd-MnO spinel catalysts with uniform morphology and active component dispersion. Among these, 1.08Pd-MnO presented the highest catalytic efficiency with a T value of 240 °C, which was 94 °C lower than that of MnO. Characterization and density functional theory (DFT) calculation results revealed that the strong metal-support interaction (SMSI) effect between Pd and MnO promoted the redistribution of surface charges, thus strengthening the oxidation-reduction ability of the active sites. Moreover, the SMSI effect led to a better migration of surface oxygen species, and boosted the generation of active surface oxygen species. Simultaneously, the Pd catalyst further reduced the energy barrier in the initial stage of the dehydrogenation of propane. Overall, this study provided a novel design strategy for dual active components catalysts with SMSI effect and extended the application of these catalysts in the important field of VOCs elimination.

摘要

调节双活性组分之间的相互作用以增强挥发性有机化合物(VOCs)的降解是一种有效的但仍具有挑战性的空气污染控制手段。在此,采用有限热解氧化策略制备了具有均匀形貌和活性组分分散性的Pd-MnO尖晶石催化剂。其中,1.08Pd-MnO表现出最高的催化效率,T值为240℃,比MnO的T值低94℃。表征和密度泛函理论(DFT)计算结果表明,Pd与MnO之间的强金属-载体相互作用(SMSI)效应促进了表面电荷的重新分布,从而增强了活性位点的氧化还原能力。此外,SMSI效应导致表面氧物种的迁移更好,并促进了活性表面氧物种的生成。同时,Pd催化剂进一步降低了丙烷脱氢初始阶段的能垒。总体而言,本研究为具有SMSI效应的双活性组分催化剂提供了一种新颖的设计策略,并扩展了这些催化剂在VOCs消除这一重要领域的应用。

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