4.7 Article

Enhancing catalytic performance of Cu-SSZ-13 for the NH3-SCR reaction via in situ introduction of Fe3+ with diatomite

Journal

MATERIALS CHEMISTRY FRONTIERS
Volume 5, Issue 21, Pages 7787-7795

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1qm01101d

Keywords

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Funding

  1. National Natural Science Foundation of China [21920102005, 21835002, 21621001, U1967215]
  2. 111 Project [B17020]

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The study synthesized highly crystalline Cu-SSZ-13 catalysts by introducing Fe3+-containing diatomite, which exhibited better catalytic activity and hydrothermal stability at high temperatures. The extra-framework Fe3+ in SSZ-13-D was found to suppress Cu2+ aggregation and promote the transformation of Cu(OH)(+) species during hydrothermal aging, leading to enhanced catalytic performance. This research provides insights for the development of efficient bimetallic Cu-based zeolite catalysts for NH3-SCR reactions.
The SSZ-13 zeolite supported Cu catalyst is highly efficient in eliminating NOx and introduction of Fe3+ ions can significantly improve the high-temperature activity and the hydrothermal stability of Cu-SSZ-13. However, the exact role of Fe species has not been investigated yet. In this work, we synthesized highly crystalline SSZ-13 with a silicon source of Fe3+-containing diatomite (SSZ-13-D) and silica sol (SSZ-13-S). The crystallization time of SSZ-13-D was only half that of SSZ-13-S. Investigation of the crystallization processes revealed that the intrinsic six-membered ring in diatomite was responsible for the significant shortening of the crystallization time. The fresh Cu-SSZ-13-D exhibited better catalytic activity than the fresh Cu-SSZ-13-S from 175-500 degrees C, especially at 200 degrees C, where the NO conversion of Cu-SSZ-13-D was 10% higher than that of Cu-SSZ-13-S. After hydrothermal ageing, the temperature window of T-90 for Cu-SSZ-13-D_HTA was narrowed to 250-350 degrees C, while the maximum NO conversion of aged Cu-SSZ-13-S_HTA was reduced to 88%. TEM, XPS, EPR, UV-Vis DRS, NH3-TPD, and H-2-TPR characterization demonstrated that the extra-framework Fe3+ in SSZ-13-D could suppress the aggregation of Cu2+ in the fresh Cu-SSZ-13-D at high reaction temperature and promoted the transformation of Cu(OH)(+) species to Cu2+ during the hydrothermal ageing leading to a better catalytic performance. The investigation of the role of Fe species in enhancing the catalytic performance of the Cu-SSZ-13 catalyst provides guidance for the preparation of efficient bimetallic Cu-based zeolite catalysts for the NH3-SCR reaction.

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