4.8 Article

Dual Promotional Effects of TiO2-Decorated Acid-Treated MnOx Octahedral Molecular Sieve Catalysts for Alkali-Resistant Reduction of NOx

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 12, Pages 11507-11517

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b01291

Keywords

octahedral molecular sieves; TiO2 decoration; alkali resistant; selective catalytic reduction; environmental catalysis

Funding

  1. National Natural Science Foundation of China [21722704, 21773152]
  2. Science and Technology Commission of Shanghai Municipality [17230741400, 15DZ2281400]
  3. China Postdoctoral Science Foundation [2018M630426]

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Alkali metals generated during waste incineration in power stations are not conducive to the control of nitrogen oxide (NOx) emission. Hence, improved selective catalytic reduction of NOx with ammonia (NH3-SCR) in the presence of alkali metals is a major issue for practical NO removal. In this work, we developed a novel TiO2-decorated acid-treated MnOx octahedral molecular sieve (OMS-5(H)@TiO2) catalyst with improved alkali-resistant NOx reduction at low temperature, and the dual promotional effects of OMS-5(H)@TiO2 catalysts were clarified. It was found that the special structure of the acid-treated MnOx octahedral molecular sieve (OMS-5(H)) was responsible for the trapping of alkali metals and high deNO(x) activity at low temperature. Subsequently, the decoration by TiO2 further improved the redox properties by accelerating the high ratio of Mn4+ and O-alpha on the surface of the highly active (OMS-S(H)@TiO2) catalyst. Moreover, a thorough mechanism study via in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs) demonstrated that the acid treatment led to remarkable increment of acid sites, which enabled the catalyst to resist alkali metals in the form of ion exchange. Meanwhile, the decoration of TiO2 further increased the strength of the Lewis acid sites, assisting more active intermediate species to effectively take part in the deNO(x) reaction. Besides, a fast SCR process was observed to certify that the decoration of TiO2 promoted the improvement of low-temperature activity in the presence of alkali metals. The dual effects combining OMS-5(H) with TiO2 decoration in terms of alkali metal resistance and high catalytic activity at low temperature proved that the high-performance deNO(x) catalyst was successfully developed in this work. The work paves a way for the development of superior low-temperature SCR catalysts with improved NOx reduction efficiency in the presence of alkali metals.

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