4.8 Article

A Novel Redox Precipitation to Synthesize Au-Doped alpha-MnO2 with High Dispersion toward Low-Temperature Oxidation of Formaldehyde

期刊

ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 52, 期 8, 页码 4728-4737

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.7b06039

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资金

  1. National Natural Science Foundation of China [21501175]
  2. Nature Science Foundation of Fujian Province of China [2016J01079, 2016J05049]
  3. Cooperation of Industry-University-Institute and Scientific and Technological Cooperation of Xiamen [3502Z20172025]
  4. One Hundred Talent Project from Chinese Academy of Sciences
  5. Xiamen High-level Overseas Innovation Talent from Xiamen
  6. Key Research Program of Frontier Sciences from Chinese Academy of Sciences [QYZDB-SSW-DQC022]

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A novel method of redox precipitation was applied for the first time to synthesize a Au-doped alpha-MnO2 catalyst with high dispersion of the Au species. Au nano particles (NPs) can be downsized into approximate single atoms by this method, thereby realizing highly efficient utilization of Au element as well as satisfying low-temperature oxidation of formaldehyde (HCHO). Under catalysis of the optimal 0.25% Au/alpha-MnO2 catalyst, a polluted stream containing 500 ppm HCHO can be completely cleaned at 75 degrees C with the condition of a weight hourly space velocity (WHSV) of 60000 mL/(g h). Meanwhile, the catalyst retains good activity for removal of low-concentration HCHO (about 1 ppm) at ambient temperature with a high WHSV, and exhibits a high tolerance to water and long-term stability. Our characterization of Au/alpha-MnO2 and catalytic performance tests clearly demonstrate that the proper amount of Au doping facilitates formation of surface vacancy oxygen, lattice oxygen, and charged Au species as an active site, which are all beneficial to catalytic oxidation of HCHO. The oxidation of HCHO over Au-doped alpha-MnO2 catalyst obeys the Mars-van Krevelen mechanism as evidenced by in situ diffuse reflectance infrared Fourier transform spectroscopy.

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