Interplay between copper redox and transfer and support acidity and topology in low temperature NH3-SCR

Yiqing Wu, Wenru Zhao, Sang Hyun Ahn, Yilin Wang, Eric D. Walter, Ying Chen, Miroslaw A. Derewinski, Nancy M. Washton, Kenneth G. Rappé, Yong Wang, Donghai Mei (), Suk Bong Hong () and Feng Gao ()
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Yiqing Wu: Pacific Northwest National Laboratory
Wenru Zhao: Tiangong University
Sang Hyun Ahn: Division of Environmental Science and Engineering, POSTECH
Yilin Wang: Pacific Northwest National Laboratory
Eric D. Walter: Pacific Northwest National Laboratory
Ying Chen: Pacific Northwest National Laboratory
Miroslaw A. Derewinski: Pacific Northwest National Laboratory
Nancy M. Washton: Pacific Northwest National Laboratory
Kenneth G. Rappé: Pacific Northwest National Laboratory
Yong Wang: Pacific Northwest National Laboratory
Donghai Mei: Tiangong University
Suk Bong Hong: Division of Environmental Science and Engineering, POSTECH
Feng Gao: Pacific Northwest National Laboratory

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Low-temperature standard NH3-SCR over copper-exchanged zeolite catalysts occurs on NH3-solvated Cu-ion active sites in a quasi-homogeneous manner. As key kinetically relevant reaction steps, the reaction intermediate CuII(NH3)4 ion hydrolyzes to CuII(OH)(NH3)3 ion to gain redox activity. The CuII(OH)(NH3)3 ion also transfers between neighboring zeolite cages to form highly reactive reaction intermediates. Via operando electron paramagnetic resonance spectroscopy and SCR kinetic measurements and density functional theory calculations, we demonstrate here that such kinetically relevant steps become energetically more difficult with lower support Brønsted acid strength and density. Consequently, Cu/LTA displays lower Cu atomic efficiency than Cu/CHA and Cu/AEI, which can also be rationalized by considering differences in their support topology. By carrying out hydrothermal aging to eliminate support Brønsted acid sites, both CuII(NH3)4 ion hydrolysis and CuII(OH)(NH3)3 ion migration are hindered, leading to a marked decrease in Cu atomic efficiency for all catalysts.

Date: 2023
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DOI: 10.1038/s41467-023-38309-8

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