Issue 8, 2018

Effect of Al-distribution on oxygen activation over Cu–CHA

Abstract

Cu(NH3)2+-pairs in chabazite (CHA) have been suggested to activate oxygen during low-temperature selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR). As charge neutrality requires that each Cu-complex is associated with a framework Al, the Al-distribution may affect Cu(NH3)2+-pair formation and subsequent oxygen activation. Here, density functional theory calculations in combination with ab initio molecular dynamics simulations are used to explore Cu(NH3)2+-pair formation and oxygen activation in Cu–CHA. The Al-distribution is found to markedly affect the probability for Cu(NH3)2+-pair formation. Moreover, the molecular dynamics simulations reveal a low-energy reaction path for O2 activation and dissociation. The facile O2 dissociation suggests that Cu-pair formation rather than O2 activation governs the low-temperature NH3-SCR activity. The results indicate that precise synthesis of Cu-exchanged chabazite with respect to Al-distribution may enhance the catalytic activity.

Graphical abstract: Effect of Al-distribution on oxygen activation over Cu–CHA

Supplementary files

Article information

Article type
Paper
Submitted
12 Jan 2018
Accepted
21 Mar 2018
First published
22 Mar 2018
This article is Open Access
Creative Commons BY-NC license

Catal. Sci. Technol., 2018,8, 2131-2136

Effect of Al-distribution on oxygen activation over Cu–CHA

L. Chen, H. Falsig, T. V. W. Janssens, J. Jansson, M. Skoglundh and H. Grönbeck, Catal. Sci. Technol., 2018, 8, 2131 DOI: 10.1039/C8CY00083B

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