HUSCAP logo Hokkaido Univ. logo

Hokkaido University Collection of Scholarly and Academic Papers >
Institute for Catalysis >
Peer-reviewed Journal Articles, etc >

Mechanistic insights into the oxidation of copper(i) species during NH3-SCR over Cu-CHA zeolites : a DFT study

Files in This Item:
MS_NH3-SCR_Cu-CHA DFT Catal Sci Technol for HUSCAP.pdf663.34 kBPDFView/Open
Please use this identifier to cite or link to this item:

Title: Mechanistic insights into the oxidation of copper(i) species during NH3-SCR over Cu-CHA zeolites : a DFT study
Authors: Liu, Chong Browse this author
Kubota, Hiroe Browse this author
Toyao, Takashi Browse this author →KAKEN DB
Maeno, Zen Browse this author →KAKEN DB
Shimizu, Ken-ichi Browse this author →KAKEN DB
Issue Date: 7-Jun-2020
Publisher: Royal Society of Chemistry
Journal Title: Catalysis science and technology
Volume: 10
Issue: 11
Start Page: 3586
End Page: 3593
Publisher DOI: 10.1039/d0cy00379d
Abstract: Selective catalytic reduction of nitrogen oxides using ammonia (NH3-SCR) over Cu-exchanged zeolites proceeds via reduction of Cu(ii) to Cu(i) and subsequent reoxidation of Cu(i) to Cu(ii). Although the mechanism of reduction half cycle has been relatively well established, reoxidation pathways of Cu(i) to form the original Cu(ii) species are highly complicated and remain unclear. Herein, oxidation mechanisms of Cu(i) to Cu(ii) species in CHA zeolites during the NH3-SCR process were investigated by periodic DFT calculations. The NH3-solvated Cu(i) and Cu(ii) species were considered for exploring the oxidative activation reaction pathways. The results show that, with O-2 as the sole oxidant, Cu(i) can be effectively oxidized to Cu(ii) via multinuclear Cu-oxo intermediates with moderate reaction barriers. The NO-assisted oxidation of Cu(i) was found to favor the formation of Cu nitrate/nitrite species, which seem to only act as off-cycle resting states. We propose that reoxidation of Cu(i) to Cu(ii) with O-2 as the sole oxidant plays a key role in the oxidation half cycle under standard NH3-SCR conditions.
Type: article (author version)
Appears in Collections:触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 鳥屋尾 隆

Export metadata:

OAI-PMH ( junii2 , jpcoar_1.0 )

MathJax is now OFF:


 - Hokkaido University