Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 10, Issue 11, Pages 3586-3593Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cy00379d
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Funding
- Japan Ministry of Economy, Trade and Industry
- JST-CREST project [JPMJCR17J3]
- KAKENHI from the JSPS [17H01341, 18K14057, 18K14051]
- JSPS postdoctoral fellowship [P19059]
- MEXT projects Elements Strategy Initiative to Form Core Research Centers
- IRCCS
- Grants-in-Aid for Scientific Research [17H01341, 18K14051, 18K14057] Funding Source: KAKEN
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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.
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