4.8 Article

Toward rational design of a novel hierarchical porous Cu-SSZ-13 catalyst with boosted low-temperature NOx reduction performance

Journal

JOURNAL OF CATALYSIS
Volume 401, Issue -, Pages 309-320

Publisher

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.07.024

Keywords

Nitrogen oxide; Reduction of NOx; Hierarchical porous Cu-SSZ-13; Hydrothermal stability; SO2 resistance

Funding

  1. National Key R&D Program of China [2016YFC0205900]
  2. National Natural Science Foundation of China [21976078, 21773106]
  3. Natural Science Foundation of Jiangxi Province [20201BAB203024]
  4. National Engineering Laboratory for Mobile Source Emission Control Technology of China [NELMS2017A03]

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The hierarchically porous Cu-SSZ-13 zeolite with enriched mesopores, named Cu-SSZ-13-HP, exhibited enhanced low-temperature activity and a widened active temperature window compared to traditional Cu-SSZ-13 with only micropores. Furthermore, Cu-SSZ-13-HP showed superior hydrothermal stability and improved sulfur dioxide tolerance, making it a promising candidate for the reduction of NOx emissions from diesel vehicles at low temperatures.
Nitrogen oxide (NOx), one of the main air pollutants exhausted from diesel vehicles, is harmful to the environment and human health and has been selectively catalytically reduced to N-2 by Cu-exchanged zeolites with chabazite structures (CHA, Cu-SSZ-13). Unfortunately, the conventional Cu-SSZ-13 catalyst still has disadvantages in real applications, such as diffusion limits and micropore blocking due to formation of ammonium sulfates, especially at low reaction temperatures. Here, a highly crystalline hierarchical porous Cu-SSZ-13 zeolite (termed Cu-SSZ-13-HP) with enriched mesopores was rationally designed and prepared via a dual-template method for the first time. The novel Cu-SSZ-13-HP catalyst displayed boosted low-temperature activity (temperature of 70% conversion below 150 degrees C) and broadened active temperature window (between 175 and 500 degrees C, NOx conversion above 90%) compared with conventional Cu-SSZ-13 with only micropores. Importantly, Cu-SSZ-13-HP also exhibited superior hydrothermal stability and enhanced sulfur dioxide (SO2) tolerance, even when exposed to 100 ppm of SO2 for 4 h. The in situ diffuse reflectance infrared Fourier transform spectroscopy revealed that the NH3 selective catalytic reduction reaction might conform to the Langmuir-Hinshelwood mechanism in which ammonia (NH3) and NOx were activated by the acid and redox sites, respectively. The Cu-SSZ-13-HP catalyst developed by the dual-template strategy might be a good candidate for low-temperature reduction of NOx exhaust from diesel vehicles. (C) 2021 Elsevier Inc. All rights reserved.

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