Strikingly distinctive NH3-SCR behavior over Cu-SSZ-13 in the presence of NO2

Yulong Shan, Guangzhi He (), Jinpeng Du, Yu Sun, Zhongqi Liu, Yu Fu, Fudong Liu, Xiaoyan Shi, Yunbo Yu and Hong He ()
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Yulong Shan: Chinese Academy of Sciences
Guangzhi He: Chinese Academy of Sciences
Jinpeng Du: Chinese Academy of Sciences
Yu Sun: Chinese Academy of Sciences
Zhongqi Liu: Chinese Academy of Sciences
Yu Fu: Chinese Academy of Sciences
Fudong Liu: University of Central Florida
Xiaoyan Shi: Chinese Academy of Sciences
Yunbo Yu: Chinese Academy of Sciences
Hong He: Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Commercial Cu-exchanged small-pore SSZ-13 (Cu-SSZ-13) zeolite catalysts are highly active for the standard selective catalytic reduction (SCR) of NO with NH3. However, their activity is unexpectedly inhibited in the presence of NO2 at low temperatures. This is strikingly distinct from the NO2-accelerated NOx conversion over other typical SCR catalyst systems. Here, we combine kinetic experiments, in situ 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 CuII species (fw-Cu2+ and NH3-solvated CuII with high CNs), which impedes the mobility of Cu species. The SCR reaction occurring at these CuII sites with weak mobility shows a higher energy barrier than that of the standard SCR reaction on dynamic binuclear sites. Moreover, the NO2-involved SCR reaction tends to occur at the Brønsted acid sites (BASs) rather than the CuII sites. This work clearly explains the strikingly distinctive selective catalytic behavior in this zeolite system.

Date: 2022
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DOI: 10.1038/s41467-022-32136-z

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