TY - JOUR
T1 - Enhancing catalytic performance of Cu-SSZ-13 for the NH3-SCR reaction
T2 - Via in situ introduction of Fe3+with diatomite
AU - Chen, Mengyang
AU - Wei, Yingzhen
AU - Han, Jinfeng
AU - Yan, Wenfu
AU - Yu, Jihong
N1 - Publisher Copyright:
© the Partner Organisations.
PY - 2021/11/7
Y1 - 2021/11/7
N2 - 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 °C, especially at 200 °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 T90 for Cu-SSZ-13-D_HTA was narrowed to 250-350 °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 H2-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.
AB - 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 °C, especially at 200 °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 T90 for Cu-SSZ-13-D_HTA was narrowed to 250-350 °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 H2-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.
UR - http://www.scopus.com/inward/record.url?scp=85118313981&partnerID=8YFLogxK
U2 - 10.1039/d1qm01101d
DO - 10.1039/d1qm01101d
M3 - Article
AN - SCOPUS:85118313981
SN - 2052-1537
VL - 5
SP - 7787
EP - 7795
JO - Materials Chemistry Frontiers
JF - Materials Chemistry Frontiers
IS - 21
ER -