Controlling Catalytic Selectivity Mediated by Stabilization of Reactive Intermediates in Small-Pore Environments: A Study of Mn/TiO2 in the NH3-SCR Reaction

ACS Catalysis ◽  
2020 ◽  
Vol 10 (20) ◽  
pp. 12017-12030
Author(s):  
Inhak Song ◽  
Hwangho Lee ◽  
Se Won Jeon ◽  
Do Heui Kim
2020 ◽  
Vol 390 ◽  
pp. 224-236 ◽  
Author(s):  
Michiel De Prins ◽  
Elke Verheyen ◽  
Andreas Hoffmann ◽  
Gina Vanbutsele ◽  
Sreeprasanth Pulinthanathu Sree ◽  
...  

2019 ◽  
Vol 575 ◽  
pp. 204-213 ◽  
Author(s):  
Yutaro Kakiuchi ◽  
Takuya Tanigawa ◽  
Nao Tsunoji ◽  
Yasuyuki Takamitsu ◽  
Masahiro Sadakane ◽  
...  

2017 ◽  
Vol 217 ◽  
pp. 125-136 ◽  
Author(s):  
Nuria Martín ◽  
Cecilia Paris ◽  
Peter N.R. Vennestrøm ◽  
Joakim R. Thøgersen ◽  
Manuel Moliner ◽  
...  

2018 ◽  
Vol 20 (17) ◽  
pp. 11976-11986 ◽  
Author(s):  
A. J. O'Malley ◽  
M. Sarwar ◽  
J. Armstrong ◽  
C. R. A. Catlow ◽  
I. P. Silverwood ◽  
...  

Neutron scattering and simulation studies reveal important consistencies and differences in ammonia mobility in small pore NH3-SCR zeolite catalysts.


2021 ◽  
Vol 281 ◽  
pp. 119480
Author(s):  
Shichao Han ◽  
Xiaomin Tang ◽  
Lijin Wang ◽  
Yanhang Ma ◽  
Wei Chen ◽  
...  

2018 ◽  
Vol 122 (45) ◽  
pp. 25948-25953 ◽  
Author(s):  
Yulong Shan ◽  
Xiaoyan Shi ◽  
Guangzhi He ◽  
Kuo Liu ◽  
Zidi Yan ◽  
...  
Keyword(s):  
Nh3 Scr ◽  

2021 ◽  
Author(s):  
Yulong Shan ◽  
Guangzhi He ◽  
Jinpeng Du ◽  
Yu Sun ◽  
Zhongqi Liu ◽  
...  

Abstract Commercial Cu-exchanged small-pore SSZ-13 (Cu-SSZ-13) zeolite catalysts are highly active for the selective catalytic reduction (SCR) of NOx with NH3, but distinct from other catalyst systems, their activity is unexpectedly inhibited in the presence of NO2. Here, we combined kinetic experiments, in-situ/operando X-ray absorption spectroscopy, and density functional theory (DFT) calculations to obtain direct evidence that under reaction conditions, strong oxidation by NO2 forces Cu ions to exist mainly as fixed framework Cu2+ species (fw-Cu2+), which impede the formation of dynamic binuclear Cu+ species that serve as the main active sites for the standard SCR (SSCR) reaction. As a result, the SSCR reaction is significantly inhibited by NO2 in the zeolite system, and the NO2-involved SCR reaction occurs with an energy barrier higher than that of the SSCR reaction on dynamic binuclear sites. Moreover, the NO2-involved SCR reaction tends to occur at the Brønsted acid sites (BAS) rather than the fw-Cu2+ sites. This work clearly explains the strikingly distinctive selective catalytic behavior in the zeolite system.


2021 ◽  
Author(s):  
Yulong Shan ◽  
Jinpeng Du ◽  
Yan Zhang ◽  
Wenpo Shan ◽  
Xiaoyan Shi ◽  
...  

Abstract Zeolites, as efficient and stable catalysts, are widely used in the environmental catalysis field. Typically, Cu-SSZ-13 with small-pore structure shows excellent catalytic activity for selective catalytic reduction of NOx with ammonia (NH3-SCR) as well as high hydrothermal stability. This review summarizes major advances in Cu-SSZ-13 applied to the NH3-SCR reaction, including the state of copper species, standard and fast SCR reaction mechanism, hydrothermal deactivation mechanism, poisoning resistance, and synthetic methodology. The review gives a valuable summary of new insights on the matching between SCR catalyst design principles and the characteristics of Cu2+-exchanged zeolitic catalysts, highlighting the significant opportunity presented by zeolite-based catalysts. Principles for designing zeolites with excellent NH3-SCR performance and hydrothermal stability are proposed. On the basis of these principles, more hydrothermally stable Cu-AEI and Cu-LTA zeolites are elaborated as well as other alternative zeolites applied to NH3-SCR. Finally, we call attention to the challenges facing Cu-based small-pore zeolites that still need to be addressed.


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