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Environmental water-mediated dual-mechanism regulation of PtCuδ-MnOx-catalyzed acetone oxidation: Enhancement of MvK and inhibition of L-H mechanism

Journal 2024 · IF 7.4 · 发表于 2024 年 8 月 25 日
作者: Lei Wang,Xin Zhang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Li Zhu,Song Qiao,Jing Ma,Jinpeng Wei,Feng Lin
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摘要

Environmental H 2 O has a significant effect on the reaction mechanism and process of VOC oxidation, of which the intrinsic mechanism is hardly reported. Herein, a series of PtCu δ -MnO x catalysts with different strong metal-supported interactions were constructed by replacing some Pt species with Cu species. Among them, the PtCu 3 -MnO x catalyst exhibited superior catalytic performance (T 90 = 170 ℃), high water resistance, and long-term stability. Furthermore, in-situ diffuse reflectance infrared Fourier transform spectroscopy ( in-situ DRIFTs) showed that the acetone oxidation followed synergistic cooperation of the Langmuir-Hinshelwood (L-H) and Mars van Krevelen (MvK) mechanism. Acetone oxidation over PtCu 3 -MnO x occurred via the L-H mechanism producing surface acetate and formate species intermediate. Above 100 °C, adsorbed acetone (i.e., acetate and formate species) reacts with MnO x lattice oxygen according to the MvK mechanism to form CO 2 and H 2 O. When water vapor was present, the L-H mechanism was impaired, inhibiting the deep oxidation of acetone. This research provides an in-depth exploration of how water vapor impacts the reaction mechanism of acetone oxidation. It offers valuable insights for creating dependable catalysts suitable for use in various industrial settings.

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