4.6 Article

Optimized Design Method for Pt/SiO2-Al2O3 with High NH3-SCO Activity and Thermal Stability

期刊

ACS OMEGA
卷 7, 期 4, 页码 3177-3184

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsomega.1c03780

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资金

  1. China Postdoctoral Science Foundation [2021M693813]
  2. Natural Science Foundation of Guangxi [2020GXNSFBA297029]
  3. Foundation of Key Laboratory of New Processing Technology for Nonferrous Metal & Materials, Ministry of Education/Guangxi Key Laboratory of Optical and Electronic Materials and Devices, Guilin University of Technology [20AA-13]

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This study systematically investigated the differences between Pt/SiO2-Al2O3 catalysts prepared by the traditional impregnation method and the strong electrostatic adsorption process. It was found that the catalyst prepared through the strong electrostatic adsorption process had smaller Pt particle size, better dispersion, and better catalytic activity and thermal stability.
Pt/SiO2-Al2O3 catalysts were prepared by the traditional impregnation method (IM) and the strong electrostatic adsorption (SEA) process. Differences in particle size, surface chemical state, Pt adsorption site, ammonia oxidation activity, and thermal stability of Pt species were studied systematically. For the fresh catalyst of Pt/SiO2-Al2O3-IM (Pt/SiO2-Al2O3-IM-fresh), Pt species were dispersed unselectively on SiO2-Al2O3, and the large average size (6.6 nm) of Pt species could be observed in a bimodal distribution (ranges of 5.5-6.5 and 8.5-9.5 nm). After the hydrothermal treatment, the Pt size of the aged catalyst (Pt/SiO2-Al2O3 IM-aged) increased significantly, especially Pt particles on SiO2 showed obvious agglomeration and some even increased to 40 nm. Conversely, for the catalyst prepared through the SEA process, Pt species of Pt/SiO2-Al2O3-SEA-fresh were selectively absorbed on Al2O3, the Pt particle size was in the range of 1.5-6.0 nm, and the average particle size was only 2.7 nm. After hydrothermal aging, Pt species did not show obvious agglomeration (the average particle size was 3.2 nm). Above all, Pt/SiO2-Al2O3-SEA presented better catalytic activity and thermal stability than Pt/SiO2-Al2O3-IM, i.e., the temperatures of 50% NH3 conversion for the fresh and aged Pt/SiO2-Al2O3-SEA catalysts were 216 and 223 degrees C, respectively, much lower than those for Pt/SiO2-Al2O3-IM-fresh (228 degrees C) and Pt/SiO2-Al2O3-IM-aged (250 degrees C).

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