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A novel viewpoint on the surface adsorbed oxygen and the atom doping in the catalytic oxidation of toluene over low-Pt bimetal catalysts
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2020-11-06 , DOI: 10.1016/j.apcata.2020.117913
Yankun Du , Jianwu Zou , Yang Guo , Xiang Xu , Hongyu Chen , Changqing Su , Zheng Zeng , Liqing Li

The low-Pt bimetal compounds (PtNi3-C and PtFe3-C) were synthesized via the chemical reduction method and the toluene catalytic oxidation experiments were conducted to test their catalytic performance. The sample of PtFe3-C (T100 = 255 ℃) possessed a better low-temperature catalytic activity than PtNi3-C (T100 = 288 ℃) due to a higher content of Pt (0), while both two catalysts had a desirable catalytic stability (⁓100 % within 72 h). The reaction kinetic parameters were acquired from the Mars-van Krevelen (MVK) model, and the MVK mechanism combined with the in-situ DRIFT was used to investigate the reaction pathway. Moreover, the theoretical calculations based on DFT was applied to study the accessibility of toluene to the surface of metal atoms doping. Herein, this study not only can provide a promising catalyst with the superior low-temperature catalytic activity and stability, but also can give a comprehensive understanding on the toluene catalytic oxidation mechanism over bimetal catalysts.



中文翻译:

低铂双金属催化剂上甲苯催化氧化过程中表面吸附氧和原子掺杂的新观点

通过化学还原法合成了低铂双金属化合物(PtNi 3 -C和PtFe 3 -C),并进行了甲苯催化氧化实验,以测试其催化性能。PtFe 3 -C(T 100  = 255℃)样品具有比PtNi 3 -C(T 100 Pt(0)含量较高,因此= 288℃),而两种催化剂均具有理想的催化稳定性(72 h内⁓100%)。从Mars-van Krevelen(MVK)模型获取反应动力学参数,并使用MVK机理与原位DRIFT相结合来研究反应路径。此外,基于DFT的理论计算被用于研究甲苯对金属原子掺杂表面的可及性。在此,本研究不仅可以提供一种具有优异的低温催化活性和稳定性的有前途的催化剂,而且可以提供对甲苯催化比双金属催化剂催化氧化机理的全面理解。

更新日期:2020-11-15
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